| 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
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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
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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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