| 1. |
- Ba, Kun, et al.
(författare)
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Billiard Catalysis at Ti3C2 MXene/MAX Heterostructure for Efficient Nitrogen Fixation
- 2022
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Ingår i: Applied Catalysis B. - : Elsevier BV. - 0926-3373 .- 1873-3883. ; 317, s. 121755-
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Tidskriftsartikel (refereegranskat)abstract
- Electrocatalytic ammonia (NH3) conversion under ambient atmosphere is crucial to mimic the nature's nitrogen cycle. But currently it is always interrupted by the HER process which is more competitive. Herein, we tactically cultivate a series of incompletely etched Ti3AlC2 MAX / Ti3C2 MXene based heterostructure catalysts whose composition can be finely tuned through regulation of the LiF percentage in mixed chemical etching agent. Notably, the surface potential difference between MAX and MXene is ~40 mV, indicating that the electron can be readily transferred from MAX to MXene across the interfaces, which is favorable for N2 fixation, yielding an outstanding Faradic efficiency of 36.9%. Furthermore, density functional theory calculations reveal the billiard-like catalysis mechanism, where the intermediates are alternatively adsorbed on MAX or MXene surfaces. Meanwhile, the rate-determining step of *NH → *NH2 possesses an energy barrier of 0.96 eV on the hetero-interface which follows associative distal mechanism. This work opens a new frontier of heterostructured catalyst for balancing electrical conductivity and catalytic activity in electrocatalysis.
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| 2. |
- Bello, Estefania, et al.
(författare)
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NH3-SCR catalysts for heavy-duty diesel vehicles : Preparation of CHA-type zeolites with low-cost templates
- 2022
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Ingår i: Applied Catalysis B. - : Elsevier BV. - 0926-3373 .- 1873-3883. ; 303
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Tidskriftsartikel (refereegranskat)abstract
- Computer-assistance allows selecting the most adequate low-cost organic structure directing agents (OSDAs) for the crystallization of Al-rich CHA-type zeolites. The host-guest stabilization energies of tetraethylammonium (TEA), methyltriethylammonium (MTEA) and dimethyldiethylammonium (DMDEA), in combination with Na, were first theoretically evaluated. This ab-initio analysis reveals that two TEA show a serious steric hindrance in a cha cavity, whereas two MTEA would present excellent host-guest confinements. The synthesis of Al-rich CHA-type zeolites has been accomplished using TEA and MTEA. Electron diffraction and high-resolution transmission electron microscopy reveal large CHA-domains with narrow faulted GME-domains in the CHAtype material synthesized with TEA, confirming the better OSDA-directing roles of MTEA cations towards the cha cavity, in good agreement with DFT calculations. Cu-exchanged Al-rich CHA-type samples achieved with MTEA and TEA show excellent catalytic activity and hydrothermal stability for the selective catalytic reduction (SCR) of NOx with ammonia under conditions relevant for future heavy duty diesel conditions.
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| 3. |
- Bergman, Susanna L., et al.
(författare)
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In-situ studies of oxidation/reduction of copper in Cu-CHA SCR catalysts: Comparison of fresh and SO2-poisoned catalysts
- 2020
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Ingår i: Applied Catalysis B: Environmental. - : Elsevier BV. - 0926-3373 .- 1873-3883. ; 269
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Tidskriftsartikel (refereegranskat)abstract
- SO2-poisoning results in deactivation of Cu-CHA SCR under standard SCR conditions; however regeneration at 700 °C completely restores the SCR performance. To understand the nature of these effects, Cu-species in the fresh and poisoned catalysts were characterized by in-situ temperature-dependent time-resolved Cu K-edge X-ray absorption spectroscopy using the multivariate curve resolution alternating least squares (MCR-ALS) approach and continuous Cauchy wavelet transforms. The extracted chemically-meaningful reference spectra of Cu-species were analyzed by DFT-assisted XANES calculations. Cu-bisulfates were found as the most energetically favorable poisoned Cu-species. The response of Cu-species to a reducing environment differs in the fresh and SO2-poisoned catalysts. Differences in reducibility are related to the formation of quasi-linear Cu-complexes in the SO2-poisoned catalyst formed during heating in H2/He. Heating in H2/He leads to partial desulfurization of the poisoned catalyst. Cooling in H2/He after heating results in more facile formation of Cu-metal clusters in fresh catalyst than in SO2-poisoned.
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| 4. |
- Chen, Lu, et al.
(författare)
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Sulfur and potassium co-doped graphitic carbon nitride for highly enhanced photocatalytic hydrogen evolution
- 2020
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Ingår i: Applied Catalysis B. - : Elsevier BV. - 0926-3373 .- 1873-3883. ; 273
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Tidskriftsartikel (refereegranskat)abstract
- Modifying the structure of a photocatalyst to tailor its electronic and physicochemical properties is an effective approach for efficient photocatalysis. Herein, we demonstrate that co-doping non-metal (S) and metal (K) atoms into graphitic carbon nitride (g-C3N4) provides excellent visible-light photocatalytic hydrogen production activity of 8.78 mmol g−1 h−1, which is 98 times higher than that of pristine g-C3N4 (0.09 mmol g−1 h−1). The apparent quantum efficiency of the S+K-co-doped g-C3N4 reaches 70 % at 420 nm. This outstanding photocatalytic performance attributed to an increased specific surface area from 6.78 to 74.23 cm3 g−1, which reduced the recombination of photogenerated charge carriers and enhanced conductivity. Various characterizations are undertaken to elucidate the S+K-co-doped g-C3N4 photocatalytic mechanism. Our work not only demonstrates a facile, eco-friendly and scalable strategy for the synthesis of S+K-co-doped g-C3N4 photocatalysts, but also opens a new avenue for the design of co-doped photocatalysts.
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| 5. |
- Dan, Meng, et al.
(författare)
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Beyond hydrogen production : Solar−driven H2S−donating value−added chemical production over MnxCd1−xS/CdyMn1−yS catalyst
- 2021
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Ingår i: Applied Catalysis B: Environmental. - : Elsevier BV. - 0926-3373. ; 284
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Tidskriftsartikel (refereegranskat)abstract
- Simultaneous hydrogen (H2) evolution and value−added chemicals production are highly attractive but have not drawn enough attention. Here, we demonstrate a hydrogen sulphide (H2S)−induced product−targeting (HIPT) strategy for the coproduction of H2 and valuable chemical feedstocks from Na2S/Na2SO3 via overall H2S splitting using a MnxCd1−xS/CdyMn1−yS catalyst driven by visible light excitation. With this chemistry, 113 mmol g−1 h−1 of hydrogen evolution rate is achieved, surpassing most of the previously reported state-of-the-art photocatalyst, together with the production of value−added Na2S2O3 with nearly 100% selectivity. This work not only provides a good example for solar energy conversion via overall H2S splitting, but also offers new insights into the resource utilization of sacrificial donor (Na2S/Na2SO3) in various catalytic fields such as H2O splitting and CO2 reduction.
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| 6. |
- Elsayed, Mohamed Hammad, et al.
(författare)
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Visible-light-driven hydrogen evolution using nitrogen-doped carbon quantum dot-implanted polymer dots as metal-free photocatalysts
- 2021
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Ingår i: Applied Catalysis B: Environmental. - : Elsevier BV. - 0926-3373. ; 283
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Tidskriftsartikel (refereegranskat)abstract
- Given the photocatalytic properties of semiconducting polymers and carbon quantum dots (CQDs), we report a new structure for a metal-free photocatalytic system with a promising efficiency for hydrogen production through the combination of an organic semiconducting polymer (PFTBTA) and N-doped carbon quantum dots (NCQDs) covered by PS-PEGCOOH to produce heterostructured photocatalysts in the form of polymer dots (Pdots). This design could provide strong interactions between the two materials owing to the space confinement effect in nanometer-sized Pdots. Small particle size NCQDs are easy to insert inside the Pdot, which leads to an increase in the stability of the Pdot structure and enhances the hydrogen evolution rate by approximately 5-fold over that of pure PFTBTA Pdots. The photophysics and the mechanism behind the catalytic activity of our design are investigated by transient absorption measurement, demonstrating the role of NCQDs to enhance the charge separation and the photocatalytic efficiency of the PFTBTA Pdot.
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| 7. |
- Granestrand, Jonas, 1988-, et al.
(författare)
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Assessment of the impact of trace elements in FAME biodiesel on diesel oxidation catalyst activity after full lifetime of operation in a heavy-duty truck
- 2024
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Ingår i: Applied Catalysis B. - Amsterdam : Elsevier. - 0926-3373 .- 1873-3883.
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Tidskriftsartikel (refereegranskat)abstract
- FAME biodiesel contains some trace amounts of Na, K, P, Ca and Mg. A diesel oxidation catalyst that had been used for an entire regulatory lifetime in a heavy-duty truck was studied, to investigate whether the presence of such trace elements poisons the catalyst. The vehicle-aged catalyst contained high loadings of S, P and Na, as well as a visible layer of soot. Activity in the NO oxidation reaction was severely decreased compared to a fresh catalyst of the same type, while the CO and C3H6 oxidation reactions were less affected. Activity testing after subsequent selective trace element removal procedures was used to decouple the effect of different poisons. Sintering was observed to be the main cause of catalyst deactivation. Of the trace elements present on the catalyst, P had the largest effect on catalyst activity, while the other trace elements had little effect.
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| 8. |
- Han, Mei, et al.
(författare)
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Promoted Self-construction of β-NiOOH in Amorphous High Entropy Electrocatalysts for the Oxygen Evolution Reaction
- 2022
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Ingår i: Applied Catalysis B. - : Elsevier. - 0926-3373 .- 1873-3883. ; 301
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Tidskriftsartikel (refereegranskat)abstract
- The exploration of an efficient electrocatalyst for the oxygen evolution reaction (OER) is urgently required for sustainable renewable-energy conversion and storage. Due to the increased chemical complexity, multimetallic catalysts provide flexibility to alter their electronic and crystal structure to attain a superior intrinsic catalytic activity via synergistic effects, which is seldom accomplished using single metal catalysts. However, the high chemical complexity increases the difficulty to prepare elemental homogenous catalysts and reveal their synergistic effect during OER process, which further hinder the design of multimetallic catalysts. Here, high entropy concept is utilized to design an NiFeCoMnAl oxide with amorphous structure as OER catalyst. The direct evidence of active Ni sites is provided by the operando Raman measurements and Fe can modify oxygen intermediates binding energy on Ni sites. The X-ray photoelectron spectroscopy (XPS) and X-ray absorption spectroscopy (XAS) reveal that the incorporation of Mn can construct the electron-rich environment of active Ni center, and the relatively lower oxidation state of Ni facilitates the self-construction of β-NiOOH intermediates, which shows promoted OER activity as confirmed by density functional theory calculations. Doping Co can enhance the conductivity and doping Al leads to the formation of nanoporous structure through dealloying process, thus each component is essential for improving OER performance. The optimized NiFeCoMnAl catalyst exhibits an overpotential of 190 mV at 10 mA cm-2 in 1 M KOH solution, much superior to the ternary and quaternary counterparts. This work sheds light on understanding the origin of high entropy catalysts’ OER activity and thereby enables the rational design of multinary transition metallic catalysts.
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| 9. |
- He, Xiaoyu, et al.
(författare)
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Dual-optimization strategy engineered Ti-based metal-organic framework with Fe active sites for highly-selective CO2 photoreduction to formic acid
- 2023
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Ingår i: Applied Catalysis B. - : Elsevier BV. - 0926-3373 .- 1873-3883. ; 327
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Tidskriftsartikel (refereegranskat)abstract
- Increasing CO2 conversion efficiency over metal-organic framework (MOF) based photocatalysts is of great significance to promote the carbon capture and utilization. In this work, a dual-benefit design strategy is deployed in the synthesis of a new two-dimensional Fe/Ti-BPDC MOF photocatalyst with atomically dispersed Fe sites. This catalyst demonstrated an excellent catalytic performance in the visible-light-driven CO2 conversion to HCOOH, achieving a high yield of 703.9 μmol g-1 h-1 at a selectivity greater than 99.7%. This is attributed to the ‘dual-optimization’ achieved by this catalyst to sustain the supply of photogenerated electrons and to effectively activate CO2. Specifically, the Fe/Ti-BPDC catalyst provides a high proportion of effective photogenerated electrons for the CO2 photocatalysis process via a unique electron transfer mechanism. Meanwhile, the strong O/Fe affinity between CO2 and atomically dispersed Fe active sites not only enables a fast CO2 activation, but also dictates the intermediate reaction pathways towards high HCOOH selectivity.
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| 10. |
- Hu, Peiji, et al.
(författare)
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In-situ exsolution of FeCo nanoparticles over perovskite oxides for efficient electrocatalytic nitrate reduction to ammonia via localized electrons
- 2024
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Ingår i: Applied Catalysis B: Environmental. - 0926-3373. ; 357
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Tidskriftsartikel (refereegranskat)abstract
- FeCo nanoparticles exsolved from Co-doped Sm0.9FeO3 nanofibers with abundant oxygen vacancies (Vos) are proposed as an efficient electrocatalyst to promote nitrate reduction reaction (NITRR). Such catalyst achieves a maximum Faradaic efficiency (FE) of 90.3 % and a large NH3 yield of 17.2 mg h−1 mg−1cat. at a negatively shifted potential of −0.9 V in 0.1 M PBS with 0.1 M NaNO3, and the alloy nanoparticles socketed into nanofibers remain extremely stable during long-term electrolysis. The reaction pathway favoring the formation of NH2OH is uncovered by in situ electrochemical tests and theoretical calculations reveal the exsolution of FeCo alloy combined with the generation of Vos enhances nitrate adsorption and lowers energy increase of the potential determining step. Finite-element simulations unveil the applied current and charges are localized on the alloys along the nanofiber, which confirms the exsolved FeCo nanoparticles are the main active sites for NITRR.
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