| 1. |
- Zhao, Xue, et al.
(författare)
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Simultaneous anchoring of Ni nanoparticles and single-atom Ni on BCN matrix promotes efficient conversion of nitrate in water into high-value-added ammonia
- 2022
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Ingår i: Chemical Engineering Journal. - : Elsevier. - 1385-8947 .- 1873-3212. ; 433:Part 2
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Tidskriftsartikel (refereegranskat)abstract
- Electrochemical synthesis of ammonia driven by clean energy is expected to realize the supply of ammonia for distributed production of industry and agriculture. Here, nickel nanoparticles and nickel in the form of single atoms were simultaneously anchored on the electrochemically active carrier BCN matrix through a structured domain strategy, which realized a high-efficiency, high-value-added, conversion of nitrate in sewage. Specifically, the electrochemical nitrate reduction reaction (NIRR) driven by BCN@Ni in alkaline media achieves an ammonia yield rate as high as 2320.2 μg h−1 cm−2 (at −0.5 V vs RHE), and Faraday efficiency as high as 91.15% (at −0.3 V vs RHE). Even in neutral and acidic media, the ammonia yield rates of NIRR driven by BCN@Ni are as high as 1904.2 μg h−1 cm−2 and 2057.4 μg h−1 cm−2, respectively (at −0.4 V vs RHE). The 15NO3- isotope labeling experiment verified that the recorded ammonia all came from the electrochemical reduction of NO3– on BCN@Ni. Density functional theory (DFT) calculations show that both nano-Ni and single-atom Ni in BCN@Ni have the ability to electrochemically convert NO3– into NH3, and that the addition of BCN can further promote the NIRR on Ni.
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| 2. |
- Gao, Sanshuang, et al.
(författare)
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Selective voltammetric determination of Cd(II) by using N,S-codoped porous carbon nanofibers
- 2018
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Ingår i: Microchimica Acta. - : Springer. - 0026-3672 .- 1436-5073. ; 185
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Tidskriftsartikel (refereegranskat)abstract
- Porous carbon nanofibers codoped with nitrogen and sulfur (NFs) were prepared by pyrolysis of trithiocyanuric acid, silica nanospheres and polyacrylonitrile (PAN) followed by electrospinning. The NFs were used to modify a glassy carbon electrode (GCE) which then displayed highly sensitive response to traces of Cd(II). Compared to a bare GCE and a Nafion modified GCE, the GCE modified with codoped NFs shows improved sensitivity for Cd(II) in differential pulse anodic sweep voltammetry. The stripping peak current (typically measured at 0.81 V vs. Ag/AgCl) increases linearly in the 2.0–500 μg·L−1 Cd(II) concentration range. This is attributed to the large surface area (109 m2·g−1), porous structure, and high fraction of heteroatoms (19 at.% of N and 0.75 at.% of S). The method was applied to the determination of Cd(II) in (spiked) tap water where it gave recoveries that ranged between 96% and 103%.
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| 3. |
- Gao, Sanshuang, et al.
(författare)
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Sensitive and Selective Differential Pulse Voltammetry Detection of Cd(II) and Pb(II) Using Nitrogen-Doped Porous Carbon Nanofiber Film Electrode
- 2017
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Ingår i: Journal of the Electrochemical Society. - : Electrochemical Society. - 0013-4651 .- 1945-7111. ; 164:13, s. H967-H974
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Tidskriftsartikel (refereegranskat)abstract
- Carbon matrix materials are regarded as one of the most important electrode materials for heavy metal detection. But even so, optimization procedures of carbon nanofibers (CNFs) for tracing Cd(II) and Pb(II) remains challenging. Here, zeolitic imidazolate framework (ZIF-8)/polyacrylonitrile (PAN)-derived nitrogen-doped porous carbon nanofibers (N-PCNFs) were investigated as a new electrode material for determining the concentration of Cd(II) and Pb(II). By optimizing electrochemical conditions such as deposition potential, deposition time, pH of buffer solution, and quantity of N-PCNFs loaded on a glassy carbon electrode (GCE), the linear response curves of Cd(II) and Pb(II) could be obtained. Due to the unique structural feature and N content, the N-PCNFs possess excellent detection limits of 0.8 mu g L-1 for Cd(II) and 0.3 mu g L-1 for Pb(II) (S/N = 3). To manifest the practical use of the sensor platform the concentration of Cd(II) and Pb(II) in normal tap and waste water were monitored. According to the ICP-MS results, the calculated recovery (97.0-107%) indicates that N-PCNFs have potential as a candidate material to monitor the concentration of Cd(II) and Pb(II) in practical samples.
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| 4. |
- Hong, Jie, et al.
(författare)
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Asymmetrically coupled co single-atom and co nanoparticle in double-shelled carbon-based nanoreactor for enhanced reversible oxygen catalysis
- 2023
-
Ingår i: Chemical Engineering Journal. - : Elsevier. - 1385-8947 .- 1873-3212. ; 455
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Tidskriftsartikel (refereegranskat)abstract
- Simultaneous construction of size-asymmetric metal single atoms and nanoparticle active sites in advanced and robust carrier materials is particularly important yet challenging for efficient reversible oxygen catalysis. Herein, a facile “chemical etching/in-Situ capture” synthesis strategy was developed to fabricate a unique double-shelled carbon-based nanobox integrated with size-asymmetric Co single-atom (CoSA) and metallic Co nanoparticle (CoNP) moiety. As expected, this well-managed catalyst product yielded remarkable bifunctional electrocatalytic performances in alkaline electrolytes, with a decent half-wave potential of 0.886 V for oxygen reduction reaction (ORR) and a small overpotential of 341 mV at 10 mA/cm2 for oxygen evolution reaction (OER). Besides, this nanobox catalyst served as a cost-effective and efficient oxygen electrode in the assembled rechargeable ZABs, exceeding the mixed electrocatalyst of expensive Pt/C-RuO2, in terms of the elevated peak power density of 239 mW/cm2, the promoted specific capacity of 770 mAh/gZn, as well as the appreciable charge–discharge cycle stability. Theoretical calculations revealed that the strong interaction between the delicate CoSA site and CoNP phase, could effectively optimize the adsorption and desorption energy barriers of reaction intermediates on the designed catalyst surface, thus achieving synergistic enhancement of electrocatalytic activity towards ORR and OER. This finding affords a feasible and effective strategy to achieve highly active and durable bifunctional catalysts for both fundamental research and practical rechargeable ZABs applications.
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| 5. |
- Jiang, Ruyuan, et al.
(författare)
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A Facile Electrochemical Sensor Based on PyTS-CNTs for Simultaneous Determination of Cadmium and Lead Ions
- 2018
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Ingår i: Sensors. - : MDPI. - 1424-8220. ; 18:5
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Tidskriftsartikel (refereegranskat)abstract
- A simple and easy method was implemented for the contemporary detection of cadmium (Cd2+) and lead (Pb2+) ions using 1,3,6,8-pyrenetetrasulfonic acid sodium salt-functionalized carbon nanotubes nanocomposites (PyTS-CNTs). The morphology and composition of the obtained PyTS-CNTs were characterized using scanning electron microscopy (SEM), energy dispersive spectrometry (EDS), and X-ray photoelectron spectroscopy (XPS). The experimental results confirmed that the fabricated PyTS-CNTs exhibited good selectivity and sensitivity for metal ion-sensing owing to the insertion of sulfonic acid groups. For Cd2+ and Pb2+, some of the electrochemical sensing parameters were evaluated by varying data such as the PyTS-CNT quantity loaded on the pyrolytic graphite electrode (PGE), pH of the acetate buffer, deposition time, and deposition potential. These parameters were optimized with differential pulse anodic sweeping voltammetry (DPASV). Under the optimal condition, the stripping peak current of the PyTS-CNTs/Nafion/PGE varies linearly with the heavy metal ion concentration, ranging from 1.0 mu g L-1 to 90 mu g L-1 for Cd2+ and from 1.0 mu g L-1 to 110 mu g L-1 for Pb2+. The limits of detection were estimated to be approximately 0.8 mu g L-1 for Cd2+ and 0.02 mu g L-1 for Pb2+. The proposed PyTS CNTs/Nafion/PGE can be used as a rapid, simple, and controllable electrochemical sensor for the determination of toxic Cd2+ and Pb2+.
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| 6. |
- Jiang, Ruyuan, et al.
(författare)
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Polysulfide/Graphene Nanocomposite Film for Simultaneous Electrochemical Determination of Cadmium and Lead Ions
- 2018
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Ingår i: NANO. - : World Scientific. - 1793-2920 .- 1793-7094. ; 13:8
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Tidskriftsartikel (refereegranskat)abstract
- An integrative electroanalytical method was developed for detecting Cd2+ and Pb2+ ions in aqueous solutions. Polysulfide/graphene (RGO-S) nanocomposites were prepared and their performance as electrochemical sensors for Cd2+ and Pb2+ was evaluated. The RGO-S nanocomposite was carefully characterized by scanning electron microscopy with energy-dispersive X-ray spectrometry, transmission electron microscopy, and X-ray photoelectron spectroscopy. The as-prepared RGO-S was incorporated into a pyrolytic graphite electrode (RGO-S/PGE) and used for detecting trace amount of Cd2+ and Pb2+ by differential pulse anodic stripping voltammetry. Under optimal conditions, the stripping peak current of RGO-S/PGE varies linearly with heavy metal ion concentration in the ranges 2.0-300 mu g L-1 for Cd2+ and 1.0-300 mu g L-1 for Pb2+. The limits of detection for Cd2+ and Pb2+ were estimated to be about 0.67 mu g L-1 and 0.17 mu g L-1, respectively. The prepared electrochemical heavy-metal-detecting electrode provides good repeatability and reproducibility with high sensitivity, making it a suitable candidate for monitoring Cd2+ and Pb2+ concentrations in aqueous environmental samples.
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| 7. |
- Li, Ziyao, et al.
(författare)
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Atomic-level orbital coupling in a tri-metal alloy site enables highly efficient reversible oxygen electrocatalysis
- 2023
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry. - 2050-7488 .- 2050-7496. ; 11:5, s. 2155-2167
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Tidskriftsartikel (refereegranskat)abstract
- Complex multi-metallic alloys with ultra-small sizes have received extensive attention in the fields of Zn-air battery and water splitting, because of their unique advantages including adjustable composition, tailorable active sites, and optimizable electronic structure. In this effort, an atomic-level orbital coupling strategy is presented to effectively regulate the electronic structures of ultra-small tri-metal Fe-Co-Ni nanoalloy particles confined in an N-doped carbon hollow nanobox. As expected, the optimal nanoalloy hybrid material exhibited notable bi-functional catalytic performances toward the oxygen reduction reaction (half-wave potential of 0.902 V) and oxygen evolution reaction (1.589 V at 10 mA cm−2) with a small ΔE of 0.687 V, exceeding the precious-metal-based and many previously reported catalysts. Furthermore, the as-assembled Zn-air device also displayed a superior specific capacity of 894 mA h g−1, a maximal power density of 247 mW cm−2, and impressive durability (over 100 hours). Ultraviolet photoelectron spectroscopy and density functional theory calculations revealed that the electronic structures could be finely tuned and optimized through ternary metal alloying, resulting in a suitable d-band center and advantageous interfacial charge-transfer, which in turn could effectively reduce the involved energy barriers in the electrocatalytic process and significantly boost its intrinsic activity of reversible oxygen catalysis. Thus, this work affords an effective method for the rational creation of bi-functional non-noble-metal-based electrocatalysts for sustainable energy technology.
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| 8. |
- Nie, Zhicheng, et al.
(författare)
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Tailoring the d-band center by intermetallic charge-transfer manipulation in bimetal alloy nanoparticle confined in N-doped carbon nanobox for efficient rechargeable Zn-air battery
- 2023
-
Ingår i: Chemical Engineering Journal. - : Elsevier. - 1385-8947 .- 1873-3212. ; 463
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Tidskriftsartikel (refereegranskat)abstract
- In this effort, the electronic-structure modulation strategy through nano-alloying was rationally designed to fabricate Fe-Ni alloy particles embedded in an N-doped carbon nanobox. The as-developed catalyst outperformed the commercialized noble-metal benchmarks with a decent half-wave potential of 0.891 V for ORR and a small overpotential of 325 mV at 10 mA/cm2 for OER both in 0.1 M KOH solution. Beyond that, a highly-efficient regenerative Zn-air battery was also successfully constructed, evidenced by a small potential gap of 0.664 V (between Ej=10 and E1/2), a high specific capacity of 763 mAh/g, a large peak power density of 270 mW/cm2, and robust stability. Ultraviolet photoelectron spectroscopy and theoretical simulation confirmed that the alloying of Ni into Fe could well manipulate the electronic structure, leading to favorable intermetallic charge-transfer and then downshifting the d-band center of Fe adsorption sites, all of which help to significantly lower the reaction barriers of the involved intermediates during the electrocatalytic ORR/OER processes.
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| 9. |
- Nie, Zhicheng, et al.
(författare)
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Vacancy and doping engineering of Ni-based charge-buffer electrode for highly-efficient membrane-free and decoupled hydrogen/oxygen evolution
- 2023
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Ingår i: Journal of Colloid and Interface Science. - : Elsevier. - 0021-9797 .- 1095-7103. ; 642, s. 714-723
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Tidskriftsartikel (refereegranskat)abstract
- The realization of the membrane-free two-step water electrolysis is particularly important yet challenging for the low-cost and large-scale supply of hydrogen energy. In this effort, Co-doped Ni(OH)2 nanosheets were successfully anchored onto the nickel foam (NF) substrate through the in-situ growth of metal-organic frame material and the subsequent alkali-etching technique. Using the well-regulated Co-doping Ni(OH)2@NF electrodes as a charge mediator, electrochemical hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) were decoupled on time scales, thus affording a membrane-free two-step route for H2 and O2 productions. In this architecture, the first HER process on the cathode could be maintained for 1300 s at a current of 100 mA, while the corresponding Ni(OH)2 charge mediator was simultaneously oxidized to NiOOH, with a decent cell voltage of 1.542 V. The subsequent OER process involved a reduction/regeneration of Ni(OH)2 (from NiOOH to Ni(OH)2) and an anodic O2-production, with an operating voltage of 0.291 V. Moreover, the Ni-Zn battery assembled through the combination of NiOOH and Zn sheet could replace the second step of OER to achieve the coupling of continuous H2-production and battery discharge, thus also providing a new way for hydrogen production without an external power supply. Experiment and theoretical calculations have shown that the cobalt-doping not only improved the conductivity of the charge-buffer electrode, but also shifted its redox potential cathodically and boosted the adsorption affinity of the buffer medium to OH– ions, both contributing to promoted HER and OER activity. Therefore, this decoupled water electrolysis device affords a promising pathway to support the efficient conversion of renewables to hydrogen.
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| 10. |
- Qiao, Mengfei, et al.
(författare)
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Ni-Co bimetallic coordination effect for long lifetime rechargeable Zn-air battery
- 2020
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Ingår i: Journal of Energy Challenges and Mechanics. - : Elsevier. - 2056-9386. ; 47, s. 146-154
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Tidskriftsartikel (refereegranskat)abstract
- The development of bifunctional oxygen electrocatalysts with high efficiency, high stability, and low cost is of great significance to the industrialization of rechargeable Zn–air batteries. A widely accepted view is that the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) follow different catalytic mechanisms, and accordingly they need different active sites for catalysis. Transition metal elements have admirable electronic acceptance ability for coordinating with reactants, and this can weaken the bond energy between reactants, thus promoting the ORR or OER reactions. Herein, the ORR and OER activities of different transition metal supported nitrogen-doped carbon nanotubes were systematically studied and compared. The optimal catalyst for synchronous ORR and OER was obtained by pyrolyzing melamine, cobalt nitrate, and nickel nitrate on carbon nanotubes, called cobalt–nickel supported nitrogen-mixed carbon nanotubes (CoNi–NCNT), which were equipped with two types of high-performance active sites—the Co/Ni–N–C structure for the ORR and CoNi alloy particles for the OER—simultaneously. Remarkably, the optimized CoNi–NCNT exhibited a satisfactory bifunctional catalytic activity for both the ORR and OER. The value of the oxygen electrode activity parameter, ΔE, of CoNi–NCNT was 0.81 V, which surpasses that of catalysts Pt/C and Ir/C, and most of the non-precious metal-based bifunctional electrocatalysts reported in previous literatures. Furthermore, a specially assembled rechargeable Zn–air cell with CoNi–NCNT loaded carbon paper as an air cathode was used to evaluate the practicability. As a result, a superior specific capacity of 744.3 mAh/gZn, a peak power density of 88 mW/cm2, and an excellent rechargeable cycling stability were observed, and these endow the CoNi–NCNT with promising prospects for practical application.
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| 11. |
- Qin, Danfeng, et al.
(författare)
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An Electrochemical Sensor Based on Green gamma-AlOOH-Carbonated Bacterial Cellulose Hybrids for Simultaneous Determination Trace Levels of Cd(II) and Pb(II) in Drinking Water
- 2018
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Ingår i: Journal of the Electrochemical Society. - : ELECTROCHEMICAL SOC INC. - 0013-4651 .- 1945-7111. ; 165:7, s. B328-B334
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Tidskriftsartikel (refereegranskat)abstract
- An eco-friendly gamma-AlOOH-carbonated bacterial cellulose (gamma-AlOOH-CBC) hybrids material was fabricated by simple pyrolysis and hydrothermal treatments. The obtained hybrids possess an intrinsic 3D nanofibrous structure decorated with chaff-like gamma-AlOOH particles. Owing to the good adsorption property and conductive, gamma-AlOOH-CBC hybrids were used to modified the glass carbon electrode (GCE) for simultaneous determination of Cd(II) and Pb(II) in aqueous samples by differential pulse anodic stripping voltammetry (DPASV) method. Various parameters affected Cd(II) and Pb(II) measurement were optimized. Under the optimal conditions, the limit of detection (S/N = 3) of the gamma-AlOOH-CBC modified electrode was evaluated to be 0.17 mu g.L-1 for Cd(II) and 0.10 mu g.L-1 for Pb(II) with the linear range of the calibration curves ranged 0.5-250 mu g.L-1 for Cd(II) and Pb(II). Furthermore, the developed electrode was also successfully utilized for monitoring trace Cd(II) and Pb(II) in drinking water samples with satisfactory results.
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| 12. |
- Yalikun, Nuerbiya, et al.
(författare)
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Bacterial cellulose-based three-dimensional carbon nanofibers for the sensitive and selective determination of uric acid
- 2018
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Ingår i: Science of Advanced Materials. - : American Scientific Publishers. - 1947-2935 .- 1947-2943. ; 10:11, s. 1623-1629
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Tidskriftsartikel (refereegranskat)abstract
- In recent years, the interest in the optimization of novel nanomaterials for electrodes preparation has received tremendous attention. This article describe about develop an electrochemical sensor for to detect the uric acid (UA). Firstly, the sensing materials of carbon nanofibers (CNFs) were prepared through an economical approach under freeze-dried, mainly for CNFs were successfully synthesized through carbonized biomass green bacterial cellulose (BC) at 800 degrees C. The obtained CNFs were used to modify the glassy carbon electrode (GCE), and have an excellent electrochemical response towards the UA. Under the optimized condition, the current response of UA at the CNFs/GCE increased also the peak current linearly with the UA concentration, the limitation of detection (LOD) calculated as 0.29 mu M (S/N = 3), revealing the a high sensitivity and an broader analytical range of the as-prepared CNFs/GCE. Finally, the proposed electrochemical sensor can be used for detection of UA in human urine with the satisfactory result.
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| 13. |
- Yalikun, Nuerbiya, et al.
(författare)
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Synthesis of an iron-nitrogen co-doped ordered mesoporous carbon-silicon nanocomposite as an enhanced electrochemical sensor for sensitive and selective determination of chloramphenicol
- 2018
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Ingår i: Colloids and Surfaces B. - : Elsevier. - 0927-7765 .- 1873-4367. ; 172, s. 98-104
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Tidskriftsartikel (refereegranskat)abstract
- In this study, we developed a sensitive electrochemical sensor for the detection of chloramphenicol (CAP). An iron-nitrogen co-doped ordered mesoporous carbon-silicon nanocomposite (Si-Fe/NOMC) was prepared as follows. First, an SBA-15 surface was treated with an iron and nitrogen co-doped carbon framework obtained from the polymerization of ethylenediamine and carbon tetrachloride via the hard templating method. The mixture was then carbonized at a high temperature (900 degrees C). Finally, the Si-Fe/NOMC modified electrode was fabricated, and employed as a high-performance electrochemical sensor to trace the CAP in drug samples using the large surface area of the hetero-atoms iron, nitrogen and silicon co-doped in the porous structure. Cyclic voltammetry and differential pulse voltammetry tests were determine to assess the efficiency of the sensor. Under optimized conditions, the sensor exhibited rapid current response for CAP in a phosphate buffer solution PBS with pH 7.5. The linear concentration of CAP ranged from 1 mu M to 500 mu M, with a limit of detection of 0.03 mu M (S/N = 3). Furthermore, the electrochemical sensor was used to detect CAP in eye drop samples with satisfactory results.
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| 14. |
- Zhang, Hua, et al.
(författare)
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Dense crystalline/amorphous phosphides/oxides interfacial sites for enhanced industrial-level large current density seawater oxidation
- 2023
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Ingår i: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 17:16, s. 16008-16019
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Tidskriftsartikel (refereegranskat)abstract
- Designing high-efficiency and low-cost catalysts with high current densities for the oxygen evolution reaction (OER) is critical for commercial seawater electrolysis. Here, we present a heterophase synthetic strategy for constructing an electrocatalyst with dense heterogeneous interfacial sites among crystalline Ni2P, Fe2P, CeO2, and amorphous NiFeCe oxides on nickel foam (NF). The synergistic effect of high-density crystalline and amorphous heterogeneous interfaces effectively promotes the redistribution of the charge density and optimizes the adsorbed oxygen intermediates, lowering the energy barrier and promoting the O2 desorption, thus enhancing the OER performance. The obtained NiFeO-CeO2/NF catalyst exhibited outstanding OER catalytic activity, with low overpotentials of 338 and 408 mV required to attain high current densities of 500 and 1000 mA cm-2, respectively, in alkaline natural seawater electrolytes. The solar-driven seawater electrolysis system presents a record-setting and stable solar-to-hydrogen conversion efficiency of 20.10%. This work provides directives for developing highly effective and stable catalysts for large-scale clean energy production.
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| 15. |
- Zhang, Lei, et al.
(författare)
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Nickel-induced charge redistribution in Ni-Fe/Fe3C@nitrogen-doped carbon nanocage as a robust Mott-Schottky bi-functional oxygen catalyst for rechargeable Zn-air battery
- 2022
-
Ingår i: Journal of Colloid and Interface Science. - : Elsevier. - 0021-9797 .- 1095-7103. ; 625, s. 521-531
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Tidskriftsartikel (refereegranskat)abstract
- Designing earth-abundant and advanced bi-functional oxygen electrodes for efficient oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are extremely urgent but still ambiguous. Thus, metal-semiconductor nanohybrids were developed with functionally integrating ORR-active Ni species, OER-active Fe/Fe3C components, and multifunctional N-doped carbon (NDC) support. Expectantly, the resulted NDC nanocage embedded with Ni-Fe alloy and Fe3C particles, as assembled Mott-Schottky-typed catalyst, delivered a promoted half-wave potential of 0.904 V for ORR and a low overpotential of 315 mV at 10 mA/cm2 for OER both in alkaline media, outperforming those of commercial Pt/C and RuO2 counterparts. Most importantly, the optimized Ni-Fe/Fe3C@NDC sample also afforded a peak power density of 267.5 mW/cm2 with a specific capacity of 773.8 mAh/gZn and excellent durability over 80 h when used as the air electrode in rechargeable Zn-air batteries, superior to the state-of-the-art bi-functional catalysts. Ultraviolet photoelectron spectroscopy revealed that the introduction of Ni into the Fe/Fe3C@NDC component could well manipulate the electronic structure of the designed electrocatalyst, leading to an effective built-in electric field established by the Mott-Schottky heterojunction to expedite the continuous interfacial charge-transfer and thus significantly promote the utilization of electrocatalytic active sites. Therefore, this work provides an avenue for the designing and developing robust and durable Mott-Schottky-typed bi-functional catalysts for promising energy conversion.
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| 16. |
- Zhao, Xue, et al.
(författare)
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Copper confined in vesicle-like BCN cavities promotes electrochemical reduction of nitrate to ammonia in water
- 2021
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Ingår i: Journal of Materials Chemistry A. - : ROYAL SOC CHEMISTRY. - 2050-7488 .- 2050-7496. ; 9:41, s. 23675-23686
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Tidskriftsartikel (refereegranskat)abstract
- Electrochemical methods to convert high-concentration nitrates present in sewage into high-value-added ammonia do not just alleviate the problem of environmental pollution but also provide less energy-intensive alternatives to the Haber-Bosch process. In this work, a metal-boron organic polymer precursor was annealed at high temperature to obtain copper nanoparticles encapsulated in a vesicle-like BCN matrix (BCN@Cu). In the electrochemical reduction of nitrate (E-NIRR), this species exhibited excellent catalytic activity. Specifically, the ammonia yields of BCN@Cu under applied potentials of -0.3 V, -0.4 V, -0.5 V, and -0.6 V versus the reversible hydrogen electrode were 271.1 mu mol h(-1) mg(cat.)(-1), 354.8 mu mol h(-1) mg(cat.)(-1), 435.6 mu mol h(-1) mg(cat.)(-1), and 576.2 mu mol h(-1) mg(cat.)(-1), respectively, and the corresponding Faraday efficiencies were 86.3%, 88.0%, 89.3%, and 88.9%. Isotope labeling experiments with (NO3-)-N-15 confirmed that the detected ammonia had originated from the electrochemical reduction of NO3- on the catalyst surface. Moreover, the E-NIRR activity of BCN@Cu remained high even after using it ten consecutive times or 20 h of continuous operation, suggesting the practicality of the industrial application of BCN@Cu. The presence of copper was key in determining BCN@Cus E-NIRR activity, while the presence of boron greatly improved its catalytic performance. Furthermore, density functional theory calculations indicated that BCN does not itself promote the reaction but rather assists the dispersion of Cu nanoparticles, thereby expanding the catalysts active surface area.
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| 17. |
- Zhao, Xue, et al.
(författare)
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Two-dimensional BCN matrix inlaid with single-atom-Cu driven electrochemical nitrate reduction reaction to achieve sustainable industrial-grade production of ammonia
- 2021
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Ingår i: APPLIED MATERIALS TODAY. - : Elsevier. - 2352-9407. ; 25
-
Tidskriftsartikel (refereegranskat)abstract
- Electrochemical methods have been proven to effectively eliminate nitrates in sewage and convert them into high value-added ammonia products. Here, after annealing treatment of metal boron cluster organic polymers formed by the combination of 1,10-phenanthroline, Cu2+ and closo-[B12H12](2)(-), a Cu single-atom doped BCN (B-doped CN) with a diamond-shaped nanosheet structure was obtained. In the electrochem-ical reduction reaction of nitrate, BCN-Cu exhibits excellent catalytic activity, specifically: 1) the ammonia yield rate reached as high as 498.85 mu g h(-1) cm(-2), 1047.14 mu g h(-1) cm(-2), 1900.07 mu g h(-1) cm(-2) and 3358.74 mu g h(-1) cm(-2) at -0.3 V, -0.4 V, -0.5 V and -0.6 V vs reversible hydrogen electrode, respectively, and Faradaic efficiency is 95.90%, 97.28%, 98.23% and 97.37%; 2) after repeated use of BCN-Cu 10 times or continuous operation for 16 h, the activity against electrochemical reduction reaction of nitrate anions is almost unchanged. The (NO3-)-N-15 isotopic labeling experiment proved that the detected NH3 comes from the reduction of NO3- on BCN-Cu. Control experiments show that the presence of Cu determines whether BCN-Cu has the possibility of catalyzing electrochemical reduction reactions of nitrate, and the presence of the B element enhances the catalytic activity of BCN-Cu. Density functional calculations indicate that in the water phase the process of reducing NO3- to NH3 on Cu-0 is an exothermic reaction, and that the adsorption process of NO3- on Cu-0 is the rate-determining step.
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| 18. |
- Barzegar, Hamid Reza, et al.
(författare)
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Palladium nanocrystals supported on photo-transformed C-60 nanorods : effect of crystal morphology and electron mobility on the electrocatalytic activity towards ethanol oxidation
- 2014
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Ingår i: Carbon. - : Elsevier BV. - 0008-6223 .- 1873-3891. ; 73, s. 34-40
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Tidskriftsartikel (refereegranskat)abstract
- We report on the synthesis and decoration of high-aspect-ratio crystalline C-60 nanorods (NRs) by functionalized palladium nanoparticles with an average size of 4.78 +/- 0.66 nm. In their pristine form, C-60 NRs suffer from partial damage in the solution-based decoration process resulting in poor crystallinity. However, by modifying the NR surface via in situ photochemical transformation in the liquid state, we are able to prepare highly stable NRs that retain their crystalline structure during the decoration process. Our method thus opens up for the synthesis of highly crystalline nanocomposite hybrids comprising Pd nanoparticles and C-60 NRs. Bys measuring the electron mobility of different C-60 NRs, we relate both the effect of electron mobility and crystallinity to the final electrocatalytic performance of the synthesized hybrid structures. We show that the photo-transformed C-60 NRs exhibit highly advantageous properties for ethanol oxidation based on both a better crystallinity and a higher bulk conductivity. These findings give important information in the search for efficient catalyst support.
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| 19. |
- Bi, Zenghui, et al.
(författare)
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Highly dispersed La−O/N−C sites anchored in hierarchically porous nitrogen-doped carbon as bifunctional catalysts for high-performance rechargeable Zn−air batteries
- 2023
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Ingår i: Energy Storage Materials. - : Elsevier. - 2405-8289 .- 2405-8297. ; 54, s. 313-322
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Tidskriftsartikel (refereegranskat)abstract
- Inexpensive, high-activity bifunctional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are imperative for the development of energy storage and conversion systems. A nitrogen-doped carbon material with a micro−meso−macroporous structure doped with La (LaPNC) containing La−O/N−C active sites is prepared using SiO2 particle templating of carbon and a metal node exchange strategy. The coordination environment of La sites stabilized by two oxygen and four nitrogen atoms (LaO2N4), is further verified by X-ray absorption spectroscopy. The ORR half-wave potential reaches 0.852 V, and the OER overpotential reaches 263 mV at 10 mA cm−2. The Zn−air battery, with LaPNC as the air cathode, has a maximum power density of 202 mW cm−2 and achieves stable charge−discharge for at least 100 h without a significant increase or decrease in the charge or discharge voltages, respectively. Density functional theory calculations suggest that LaO2N4 sites exhibit the lowest activation free energy and the most easily desorbed oxygen capacity. This study provides new insights into the design of efficient, durable bifunctional catalysts as alternatives to precious-metal-based catalysts.
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| 20. |
- Bi, Zenghui, et al.
(författare)
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Three dimensional star-like mesoporous nitrogen-doped carbon anchored with highly dispersed Fe and Ce dual-sites for efficient oxygen reduction reaction in Zn-air battery
- 2022
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Ingår i: Colloid and Interface Science Communications. - : Elsevier. - 2215-0382. ; 49
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Tidskriftsartikel (refereegranskat)abstract
- Metal‑nitrogen‑carbon materials (M-N-C) have attracted much attention due to their low cost, high abundance, and efficient catalytic performance. Nevertheless, Fe-N-C materials are considered the most promising oxygen reduction reaction (ORR) catalysts for replacing noble metals. Ce is chemically active and has many metal valence states, and empty orbitals that can participate in coordination. On this basis, Fe, Ce-codoped catalyst was constructed in this study. The synergistic effect of the dual metal centers was verified, and a Fe, Ce-codoped nitrogen-doped carbon (FeCeNC) with six equal branch angles was proposed. The half-wave potential for the ORR catalyzed by FeCeNC is 0.855 V. As a rechargeable Zn-air battery cathode catalyst, FeCeNC exhibits excellent electrochemical performances, with an open-circuit voltage of 1.427 V, a maximum power density of 169.2 mW cm−2 and a stable cycling time of 80 h, demonstrating an excellent cycle performance.
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| 21. |
- Ding, Pengjia, et al.
(författare)
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NiCo2O4 hollow microsphere–mediated ultrafast peroxymonosulfate activation for dye degradation
- 2021
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Ingår i: Chinese Chemical Letters. - : Elsevier. - 1001-8417 .- 1878-5964. ; 32:8, s. 2495-2498
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Tidskriftsartikel (refereegranskat)abstract
- Morphology and dispersity are key factors for activating peroxymonosulfate (PMS). In this study, we designed a recyclable open-type NiCo2O4 hollow microsphere via a simple hydrothermal method with the assistance of an NH3 vesicle. The physical structure and chemical properties were characterized using techniques such as scanning electron microscope (SEM), transmission electron microscope (TEM), X-ray diffraction (XRD), N2 adsorption and X-ray photoelectron spectroscopy (XPS). The test results confirm that the inner and outer surfaces of open-type NiCo2O4 hollow-sphere can be efficiently utilized because of the hole on the surface of the catalyst, which can minimize the diffusion resistance of the reactants and products. Under optimized conditions, the total organic carbon (TOC) removal efficiency of rhodamine B (RhB) can reach up to 80% in 40 min, which is almost 50% shorter than the reported values. The reactive radicals were identified and the proposed reaction mechanism was well described. Moreover, the disturbances of HCO3−, NO3−, Cl− and H2PO4− were further investigated. As a result, HCO3− and NO3− suppressed the reaction while Cl− and H2PO4− had a double effect on reaction.
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| 22. |
- Fan, Xiaoyu, et al.
(författare)
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Paper test strip for silver ions detection in drinking water samples based on combined fluorometric and colorimetric methods
- 2023
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Ingår i: Arabian Journal of Chemistry. - : Elsevier. - 1878-5352 .- 1878-5379. ; 16:2
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Tidskriftsartikel (refereegranskat)abstract
- In this study, a portable silver ion (Ag+) sensor was fabricated based on a dual signal output system using black phosphorus quantum dots (BPQDs) as probes. It is the first work for Ag+ detection using paper test strip based on BPQDs. The color change of BPQDs paper sensor for the determination of Ag+ was easily identified by naked eye. BPQDs were synthesized from bulk black phosphorus (BP) by mechanical exfoliation combined with a solvothermal method. BPQDs exhibited blue fluorescence with a quantum yield of 8.82 %. The fluorescence of BPQDs can be quenched by Ag+, and the absorbance of BPQDs is increased with increasing Ag+ concentration. The mechanism of the interaction between BPQDs and Ag+ involving fluorescence quenching and bonding was investigated by experimental and computational methods. The detection limit of Ag+ was 1.56 μg/mL and 0.19 μg/mL using fluorometry and colorimetry methods, respectively. A portable visual sensor based on paper test strip was constructed for Ag+ detection using the colorimetric approach. The strategy was employed to determine Ag+ successfully in drinking water samples. Therefore, the proposed portable Ag+ sensor can be potentially utilized for the lab-free analysis of drinking water and even dietary samples.
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| 23. |
- Geng, Longlong, et al.
(författare)
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Valence-mixed CuOx-nanoparticles anchored biomass-based carbon nanofiber for boosting toxic nitroarenes reduction : Synthesis, kinetics, and mechanisms
- 2022
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Ingår i: Journal of Environmental Chemical Engineering. - : Elsevier. - 2213-3437. ; 10:6
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Tidskriftsartikel (refereegranskat)abstract
- The rational modulation of metal catalysts with tailorable valence and redox properties is a promising strategy for further improving their catalytic performance. Herein, an environment-friendly grafting and thermal strategy was adopted to immobilize copper oxides nanoparticles on carbon nanofiber (CuOx/CF). Benefiting from the defect-rich surface and valence-mixed composition of the CuOx species, the optimized sample CuOx/CF-3 exhibits superb activity for the catalytic reduction of toxic nitrophenols. The complete conversion took only 1 min and an outstanding rate constant (k) of 112.7 × 10-3 s-1 was achieved under mild conditions (25 °C and 1 atm). Kinetic and recycle experiments demonstrated that the whole catalytic process obeys a pseudo-order kinetic, and the catalyst could maintain high conversion even after 13 successive recycles. These results demonstrate that CuOx/CF-3 is an alternative catalyst to noble metals, providing superb catalytic efficiency and stability in the reduction of toxic nitrophenols, and it can be expanded to develop other noble-metal-free catalysts for various applications.
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| 24. |
- Gracia-Espino, Eduardo, et al.
(författare)
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Understanding the Interface of Six-Shell Cuboctahedral and Icosahedral Palladium Clusters on Reduced Graphene Oxide : Experimental and Theoretical Study
- 2014
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 136:18, s. 6626-6633
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Tidskriftsartikel (refereegranskat)abstract
- Studies on noble-metal-decorated carbon nanostructures are reported almost on a daily basis, but detailed studies on the nanoscale interactions for well-defined systems are very rare. Here we report a study of reduced graphene oxide (rGOx) homogeneously decorated with palladium (Pd) nanoclusters with well-defined shape and size (2.3 +/- 0.3 nm). The rGOx was modified with benzyl mercaptan (BnSH) to improve the interaction with Pd clusters, and N,N-dimethylformamide was used as solvent and capping agent during the decoration process. The resulting Pd nanoparticles anchored to the rGOx-surface exhibit high crystallinity and are fully consistent with six-shell cuboctahedral and icosahedral clusters containing similar to 600 Pd atoms, where 45% of these are located at the surface. According to X-ray photoelectron spectroscopy analysis, the Pd clusters exhibit an oxidized surface forming a PdOx shell. Given the well-defined experimental system, as verified by electron microscopy data and theoretical simulations, we performed ab initio simulations using 10 functionalized graphenes (with vacancies or pyridine, amine, hydroxyl, carboxyl, or epoxy groups) to understand the adsorption process of BnSH, their further role in the Pd cluster formation, and the electronic properties of the graphene-nanoparticle hybrid system. Both the experimental and theoretical results suggest that Pd clusters interact with fiinctionalized graphene by a sulfur bridge while the remaining Pd surface is oxidized. Our study is of significant importance for all work related to anchoring of nanoparticles on nanocarbon-based supports, which are used in a variety of applications.
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| 25. |
- Han, Xin-Bao, et al.
(författare)
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Ultrasmall Abundant Metal-Based Clusters as Oxygen-Evolving Catalysts
- 2019
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 141:1, s. 232-239
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Tidskriftsartikel (refereegranskat)abstract
- The oxygen evolution reaction is a crucial step in water electrolysis to develop clean and renewable energy. Although noble metal-based catalysts have demonstrated high activity for the oxygen evolution reaction, their application is limited by their high cost and low availability. Here we report the use of a molecule-to-cluster strategy for preparing ultrasmall trimetallic clusters by using the polyoxometalate molecule as a precursor. Ultrafine (0.8 nm) transition-metal clusters with controllable chemical composition are obtained. The transition-metal clusters enable highly efficient oxygen evolution through water electrolysis in alkaline media, manifested by an overpotential of 192 mV at 10 mA cm–2, a low Tafel slope of 36 mV dec–1, and long-term stability for 30 h of electrolysis. We note, however, that besides the excellent performance as an oxygen evolution catalyst, our molecule-to-cluster strategy provides a means to achieve well-defined transition-metal clusters in the subnanometer regime, which potentially can have an impact on several other applications.
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