INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Yuehuan Zhang,Yangqin Feng,Qiang Yuan
Modulating the electronic structure of nanoclusters with high-valence metals is essential for boosting the activity of pH-universal hydrogen evolution reaction (HER) catalysts. Here, we enhance the high-valence Mo-induced strong metal-support interaction (SMSI) between anchored amorphous sub-2 nm PtRu nanoclusters and phosphomolybdic acid (H 3 PMo 12 O 40 , PMo 12 ) through a one-pot route. The optimized Pt 0 · 63 Ru 0 · 37 /PMo 12 catalyst requires overpotentials of only 27 mV (alkaline), 38 mV (neutral), and 14 mV (acidic) to drive 10 mA cm −2 . Its mass activities (9.89, 8.77, and 9.67 A mg −1 Pt + Ru ) are 3.99, 4.59, and 3.01 times higher than those of Pt/C, respectively. Structural analysis and in situ Raman experiments confirm that the electronic structure modulation between PMo 12 and PtRu clusters accelerates water adsorption/desorption, thereby enhancing HER kinetics. Finally, the assembled Pt 0 · 63 Ru 0 · 37 /PMo 12 || IrO 2 anion exchange membrane electrolyzer operates stably for over 300 h at 500 mA cm −2 . This study broadens the support selection for pH-universal water-splitting catalysts.
研究领域:
催化
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电化学
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纳米材料
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能量转换
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Nanzhu Nie,Dan Zhang,Zuochao Wang,Wenhao Yu,Shijie Ge,Juan Xiong,Yanli Gu,Bo Yang,Jianping Lai,Lei Wang
Powerful, efficient, and corrosion-resistant electrocatalysts are in need to achieve high-current-density neutral seawater hydrogen evolution. Here, a novel strategy through strong metal-support interaction (SMSI) and incorporation of Pt to construct PtNb-Nb 2 O 5 clusters @C was developed with stable high-current-density neutral seawater hydrogen evolution property for the first time. SMSI prevents agglomeration and corrosion of nanomaterials. Pt sites were proposed to play an anabranch role by binding H* to stabilize the Nb valence state and prevent water dissociation incapacitation. The optimized PtNb-Nb 2 O 5 @CC delivers low overpotentials of 440 mV (500 mA cm −2 ) and 570 mV (1000 mA cm −2 ) in neutral seawater and has 360 h excellent durability at 500 mA cm −2 . In-situ Fourier transform infrared spectroscopy (FTIR), in-situ Raman spectroscopies and theoretical calculations supported the hydrogen evolution reaction (HER) mechanism. PtNb-Nb 2 O 5 heterogeneous interface provided more active sites for water dissociation. OH* adsorbed on Nb sites in stable Nb 2 O 5 , and H* adsorbed on Nb sites and desorbed as H 2 on Pt sites in stable PtNb. Overall, this work not only first achieves stable high-current-density neutral seawater hydrogen evolution property, but also opens a new opportunity to explore SMSI and incorporation of Pt to prevent agglomeration, corrosion, and water dissociation incapacitation for catalytic applications under high current densities.
研究领域:
材料科学
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电化学
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可再生能源
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催化
✓ 已验证
DOI
高影响因子
JACS Au
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2022
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IF 0
Yuhai Sun,Junliang Wu,Yaolin Wang,Jingjing Li,Ni Wang,Jonathan Harding,Shengpeng Mo,Limin Chen,Peirong Chen,Mingli Fu,Daiqi Ye,Jun Huang,Xin Tu
Plasma-catalytic CO2 hydrogenation is a complex chemical process combining plasma-assisted gas-phase and surface reactions. Herein, we investigated CO2 hydrogenation over Pd/ZnO and ZnO in a tubular dielectric barrier discharge (DBD) reactor at ambient pressure. Compared to the CO2 hydrogenation using Plasma Only or Plasma + ZnO, placing Pd/ZnO in the DBD almost doubled the conversion of CO2 (36.7%) and CO yield (35.5%). The reaction pathways in the plasma-enhanced catalytic hydrogenation of CO2 were investigated by in situ Fourier transform infrared (FTIR) spectroscopy using a novel integrated in situ DBD/FTIR gas cell reactor, combined with online mass spectrometry (MS) analysis, kinetic analysis, and emission spectroscopic measurements. In plasma CO2 hydrogenation over Pd/ZnO, the hydrogenation of adsorbed surface CO2 on Pd/ZnO is the dominant reaction route for the enhanced CO2 conversion, which can be ascribed to the generation of a ZnOx overlay as a result of the strong metal–support interactions (SMSI) at the Pd–ZnO interface and the presence of abundant H species at the surface of Pd/ZnO; however, this important surface reaction can be limited in the Plasma + ZnO system due to a lack of active H species present on the ZnO surface and the absence of the SMSI. Instead, CO2 splitting to CO, both in the plasma gas phase and on the surface of ZnO, is believed to make an important contribution to the conversion of CO2 in the Plasma + ZnO system.
研究领域:
催化化学
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等离子体化学
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环境科学
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可持续能源
✓ 已验证
产品关联
DOI
PubMed
ACS Catalysis
·
2018
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IF 11.384
Yanfu Ma,Guangyue Xu,Hao Wang,Yingxiong Wang,Ying Zhang,Yao Fu
In this study, rare earth (RE) metal doped ZrO2 was prepared by a surfactant-assisted coprecipitation/hydrothermal crystallization method and used to load Co as catalyst for the hydrogenation of aromatic carbonyl compounds in water. Furfural was hydrogenated to furfural alcohol in water with up to 95 mol % yield over Co/ZrLa0.2Ox at 40 °C, 2 MPa H2 in 10 h. The doping of rare earth metal oxide has three advantages: (I) it promotes the ZrO2 to reach a small-sized, stable, and high-activity tetragonal phase zirconia and thus lead to a high specific surface area for metal loading; (II) it interacts with Co to reach an ultrasmall average particle size of 1.1 nm; and (III) it modifies the ZrO2 surface to increase the amount of acidic sites for the adsorption of carbonyl feedstock. The adsorption experiment indicated a tight interaction between not only the carrier and C═O bond but also the Co clusters and C═O bond, which were of benefit for the hydrogenation of carbonyl groups. The surfactant addition during the carrier preparation improves the strong metal–support interactions (SMSI) to promote Co dispersion and stability. Various rare earth metals including La, Pr, Nd, and Ce could modify ZrO2 with a similar mechanism. The as-prepared Co catalyst could also catalyze the selective hydrogenation of various aromatic aldehydes and ketones (such as 5-hydroxymethyl furfural, benzaldehyde, and acetophenone) in water, and 100% yield to corresponding alcohols was achieved. The catalyst remained stable and showed little deactivation during the recycling tests. This study not only presented a high-efficient, low-cost, and stable catalyst for the selective hydrogenation of various aromatic aldehydes and ketones but also give rise to an understanding of rare earth metal oxide doped ZrO2 supported nano Co ternary catalysts.
研究领域:
催化
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材料科学
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化学工程
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绿色化学
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）