JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
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IF 9.4
Rundong Ma,Han Tian,Xu Yu,Xiangzhi Cui,Xinmei Hou,Shengli An
Hydrogen oxidation reaction (HOR) as the anode reaction in proton exchange membrane fuel cell, usually suffers from the high loading of platinum (Pt) and subsequent CO poisoning especially by using industrial crude hydrogen as fuel. In this work, we propose a directional electron transfer route from Pt to MoO 2- x in the macroporous structure to significantly enhance the HOR activity as well as the CO tolerance, which is constructed by interface engineering and defect strategy to anchor highly dispersed Pt nanoparticles onto the three-dimensional MoO 2- x -C framework. The optimized 2Pt-MoO 2- x -C with 1.02 wt% Pt demonstrates higher HOR peak current density (3.57 mA cm −2 ) and nearly 25 times higher mass activity than 20 wt% Pt/C. The excellent HOR performance is attributed to the synergistic effect between Pt and MoO 2- x species, in which the charge transfer from Pt to MoO 2- x improves H 2 adsorption ability of Pt and accelerates the activation of H 2 due to the reduced hydrogen binding energy of MoO 2- x caused by Pt-O construction, leading to the release of H* thereby the enhancement of HOR activity. The construction of three-dimensional macroporous structure enhances the HOR dynamics by promoting the conductivity, mass transfer and the exposure of active sites. Moreover, the formed Mo-OH in Pt-MoO 2- x -C can effectively react with CO species to remove the CO poisoning of Pt, endowing the excellent CO tolerance.
研究领域:
材料科学
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电化学
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能源科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2025
·
IF 4.7
Chunli Wang,Na Yang,Dongxue Cai,Shu-Zhong Zhan,Kun Liu
The electrocatalytic processes of hydrogen evolution reaction and hydrogen oxidation reactions have emerged as global strategies to address critical environmental and energy challenges associated with fossil fuel consumption. To enhance electrocatalytic activity, we focus on the design of novel electrocatalysts based on first-row transition metal complexes. A new nickel complex [Ni(dppe)Cl 2 ] by the reaction of NiCl 2 with 1,2-bis(diphenylphosphino)ethane (dppe) were synthesized and characterized in our group. The structure of nickel complex was determined cryptographically. The electro-catalyze hydrogen evolution (HER) activity of complex Ni(dppe)Cl 2 in acetonitrile solution with acetic acid as proton and a neutral buffer (pH 7.0) medium was evaluated by controlled potential electrolysis, with a turnover frequency (TOF) of 155 and 366 (mol of H 2 /mol of cat/h), respectively. Notably, electrocatalytic activity towards hydrogen oxidation (HOR) in acetonitrile solvent using Ni(dppe)Cl 2 as a catalyst has also been studied, and the complex exhibits highly catalytic efficiency with a TOF of 0.77 s −1 . The above results indicate that the Ni complex can be act as promising electrocatalyst for HER and HOR.
研究领域:
化学
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材料科学
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能源研究
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产品关联
DOI
高影响因子
ACS Catalysis
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2019
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IF 12.221
Xueping Qin,Lulu Zhang,Gui-Liang Xu,Shangqian Zhu,Qi Wang,Meng Gu,Xiaoyi Zhang,Chengjun Sun,Perla B. Balbuena,Khalil Amine,Minhua Shao
Improving the reaction kinetics of hydrogen evolution and oxidation reactions (HER/HOR) in alkaline media is critical to promote the development of alkaline fuel cells and electrolyzers. Here, we prepared Pd3Ru alloy nanocatalysts with Ru segregated on the surfaces, forming adatoms and clusters. This structure dramatically lowered the overpotential of Pd toward HER in 1 M KOH by 104 mV at 10 mA cm–2. The HER activity was even higher than that of Pt (6 mV improvement at 10 mA cm–2). Theoretical simulation results revealed that Ru adatoms/clusters on the surface could weaken the hydrogen-binding energy and promote the OH adsorption, consequently lowering the reaction barrier of the rate-determining step in HER. Our findings are of significance for clarifying the role of Ru in bimetallic catalysts and rational design of more active catalysts for HER/HOR.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
Communications Chemistry
·
2022
·Vol. 5
·期 1
·1-8
·
IF 7.211
Xu Jiacheng,Zhang Tiantian,Fang Shiyu,Li Jing,Wu Zuliang,Wang Wei,Zhu Jiali,Gao Erhao,Yao Shuiliang
Understanding of the roles of oxygen species at reducible metal oxide surfaces under real oxidation conditions is important to improve the performance of these catalysts. The present study addresses this issue by applying a combination of operando diffuse reflectance infrared Fourier transform spectroscopy with a temperature-programmed reaction cell and mass spectrometry to explore the behaviors of oxygen species during H 2 oxidation in a temperature range of 25–400 °C at β-MnO 2 surfaces. It is revealed that O 2 is dissociated simultaneously into terminal-type oxygen (M 2+ -O 2– ) and bridge-type oxygen (M + -O 2– -M + ) via adsorption at the Mn cation with an oxygen vacancy. O 2 adsorption is inhibited if the Mn cation is covered with terminal-adsorbed species (O, OH, or H 2 O). In a temperature range of 110–150 °C, OH at Mn cation becomes reactive and its reaction product (H 2 O) can desorb from the Mn cation, resulting in the formation of bare Mn cation for O 2 adsorption and dissociation. At a temperature above 150 °C, OH is reactive enough to leave bare Mn cation for O 2 adsorption and dissociation. These results suggest that bare metal cations with oxygen vacancies are important to improve the performance of reducible metal oxide catalysts.
研究领域:
催化化学
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材料科学
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表面科学
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DOI
高影响因子
ELECTROCHIMICA ACTA
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2019
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IF 5.383
Wei Liu,Kangjie Lyu,Li Xiao,Juntao Lu,Lin Zhuang
The mechanism of hydrogen oxidation reaction (HOR) in alkaline media is still under debate. In this work, we have systemically examined the HOR performance on planar Pt electrodes modified with ten different kinds of metal hydroxides/oxides (metal = Mg, Cr, Mn, Fe, Co, Ni, Cu, Ru, La and Ce). The HOR exchange current density ( i 0 ) increases monotonically with higher electrode’s oxophilicity, which is determined by the current densities of CO stripping at 0.4 V vs. RHE ( i CO @0.4 V). However, the Ru modification exhibits a clear deviation from the monotonic relation and it demonstrates a superior catalytic activity towards HOR, relative to other metal modifications. This unexpected result is ascribed to the reduction in hydrogen binding energy (HBE) owing to the modification of metallic Ru rather than its corresponding hydroxide or oxide. The present study indicates that the electronic effect and the oxophilic effect co-exist in the HOR on Pt-based catalysts in alkaline media, but the former one is of more significance.
研究领域:
电化学
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材料科学
✓ 已验证
DOI
高影响因子
Nano Research
·
2021
·Vol. 14
·期 7
·2441-2450
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IF 8.897
Peng Lingxin,Tian Han,Cui Xiangzhi,Su Liang,Meng Ge,Ma Zhonghua,Cao Shaowen,Shi Jianlin
Developing anode catalysts of substantially enhanced activity for hydrogen oxidation reaction (HOR) and anti-CO poisoning performance is of great importance for the application of proton exchange membrane fuel cells (PEMFCs). Herein, we report Pd cluster in situ decorated urchin-like W 18 O 49 (WO 2.72 ) electrocatalysts by a photo-reduction method for high performance HOR. The synthesized Pd-WO 2.72 -L composite of low loading amount of 0.44 wt.% Pd by Xenon light reduction exhibits markedly high HOR catalytic activity and stability in 0.5 M H 2 SO 4 , and the specific HOR current density and mass activity of Pd-WO 2.72 -L are ∼ 1.5 and ∼ 80 times those of 20 wt.% Pt/C catalyst, respectively. Moreover, excellent anti-CO poisoning ability has also been obtained. The excellent HOR activity and anti-CO poisoning performance of Pd-WO 2.72 -L have been discussed mainly in terms of the dual synergetic catalytic effects between Pd and WO 2.72 : Pd activation to Pd δ+ by the electron transfer from Pd to W promotes the hydrogen adsorption and activation to H* species, which results in largely elevated HOR activity; Pd degradation due to the CO poisoning is effectively prevented by WO 2.72 , which is responsible for the excellent CO-tolerance performance.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Yuzhi Li,Janel Abbott,Yanchun Sun,Jianmin Sun,Yunchen Du,Xijiang Han,Gang Wu,Ping Xu
Here, in an effort to prepare Ru-based metal organic frameworks, we developed a one-step solvothermal synthesis for Ru nanoassembly catalysts, which consist of ˜4 nm Ru nanoparticles well dispersed on amorphous carbon (Ru/C). The Ru/C catalyst obtained from a mixed solvent of H 2 O and CH 3 CH 2 OH (Ru/C-H 2 O/CH 3 CH 2 OH), featured a chain-like porous structure, provides Pt-like catalytic properties with low overpotentials at −10 mA cm −2 for the hydrogen evolution reaction (HER) within a wide range of pH values, i.e., 35 mV in 0.5 M H 2 SO 4 , 53 mV in 1.0 M KOH, and 93 mV in 3.5 wt% NaCl. Ru/C is also an efficient hydrogen oxidation reaction (HOR) catalyst at all pH values. In the alkaline media, Ru/C-H 2 O/CH 3 CH 2 OH achieves a mass activity of 41.1 mA mg -1 at an overpotential of 50 mV and a high exchange current density (0.65 mA cm −2 ). The work provides a facile strategy to synthesize highly active Ru/C catalysts for bifunctional HER and HOR electrocatalysis.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Wanli Liang,Mengyan Zhou,Xiulan Li,Lijie Zhu,Zhixin Li,Yifan Zhou,Jian Chen,Fangyan Xie,Hao-Fan Wang,Nan Wang,Yanshuo Jin,Hui Meng
Hydrogen energy is the most suitable solution for long-term, large-scale energy storage, and the design of efficient, economical, and stable electrocatalysts for hydrogen oxidation reaction (HOR) and hydrogen evolution reaction (HER) is of great significance for its commercial development. Herein, Ni nanocluster supported on oxygen-vacancy-rich MoO 2 (Ni/MoO 2−x ) is designed which contains a large number of oxygen vacancies and Ni–O–Mo bonds. According to X-ray photoelectron spectroscopy, the formation of oxygen vacancies and Ni–O–Mo bonds facilitates the transfer of electrons from Ni to O. The prepared Ni/MoO 2−x @NF shows excellent hydrogen electrocatalytic activity, which is proved by a Tafel slope of only 26 mV dec −1 for HER and an exchange current density of 3.64 mA cm −2 for HOR. Theoretical calculations showed optimized free energy of hydrogen adsorption and hydroxide adsorption on Ni/MoO 2−x , which can explain the origin of the high activity of the catalyst. This work provides a feasible strategy for designing non-precious metal hydrogen electrocatalytic materials in energy storage.
研究领域:
材料科学
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能源存储与转换
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2025
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IF 9.5
Youpeng Cao,Hongling Liu,Yuxuan Xiao,Lun Li,Jiao Yang,Chunfa Liu,Chengcheng Zhong,Wendi Zhang,Shuyang Peng,Junge Yang,Zhichao Yu,Weng Fai Ip,Hui Pan
Platinum (Pt) is a highly efficient catalyst for the hydrogen evolution reaction (HER) and the hydrogen oxidation reaction (HOR). However, the scarcity of Pt necessitates the development of catalysts with low Pt content while maintaining high activity. In this study, we report the synthesis of oxygen-modified supra-nanometer-sized RuPt nanocrystals with low Pt content by a simple air annealing method to achieve a catalyst with high activity. The annealed catalyst, RuPt/C-200, exhibits a very low overpotential of only 3.8 mV at 10 mA cm−2, a low Tafel slope of 16.6 mV dec−1, and a 2.8-fold increase in mass activity at an overpotential of 0.06 V for HER compared to the unannealed catalyst. Additionally, the HOR exchange current density increases 2.9-fold compared to the unannealed catalyst. AEMWE tests confirm the application potential of RuPt/C-200, while density-functional-theory (DFT) calculations reveal that oxygen modification, by optimizing the hydrogen binding energy, plays a crucial role in improving the catalytic performance of RuPt. This work highlights that combining the oxygen modification strategy with the nanoscale size effect could advance the development of high-performance RuPt electrocatalyst for both alkaline HER and HOR.
研究领域:
材料科学
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电化学
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理论计算
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Mengyuan Jin,Xiang Han,Ting Chou,Shuangyan Li,Yecan Pi,Kai Chen,Tingting Chen,Shun Wang,Yun Yang,Juan Wang,Huile Jin
Developing highly efficient electrocatalyst with heterostructure for hydrogen evolution and oxidation reactions (HER/HOR) in alkaline media is crucial to the fabrication and conversion of hydrogen energy but also remains a great challenge. Herein, the synthesis of ruthenium-nickel nanoparticles (Ru 3 -Ni NPs) with heterostructure for hydrogen electrocatalysis is reported, and studies show that their catalytic activity is improved by electron redistribution caused by the distinctly heterogeneous interface. Impressively, Ru 3 -Ni NPs possess the remarkable exchange current density (2.22 mA cm −2 ) for HOR. Additionally, an ultra-low overpotential of 28 mV is required to attain a current density of 10 mA cm −2 and superior stability of 200 h for HER. The highly efficient catalytic activity can be attributed to the electron transfer from Ni to Ru and the optimal adsorption of H* on Ru-Ni sites. Our study showcases a reliable heterostructure that boosts the HOR/HER activity of the catalyst in alkaline environments. This work provides a new pathway for designing high-performance electrocatalyst for energy storage and conversion.
研究领域:
材料科学
·
能源科学
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产品关联
DOI
PubMed
高影响因子
Advanced Powder Materials
·
2025
·
IF 24.9
Xu Zhang,Peng Yu,Di Shen,Bin Cai,Tianyu Han,Ying Xie,Lei Wang
The susceptibility of Pt catalyst surfaces to carbon monoxide (CO) poisoning in anodic hydrogen oxidation reaction (HOR) has been a critical constraint on the development of proton exchange membrane fuel cells (PEMFCs). Effectively regulating the electronic structure of Pt to enhance CO resistance is crucial for developing high-performance catalysts with robust anti-poisoning capabilities. Herein, the Pt/W@NCNF features by Pt nanoparticles and atomical dispersed tungsten (W) sites on N-doped carbon nanofibers is developed for CO tolerance HOR catalyst. The presence of W enables the electron transfer from Pt, which promotes electron rearrangement in the Pt-5d orbitals. It not only optimizes the adsorption of H* and CO* on Pt, but also the OH* intermediates adsorbed on the W sites oxidize the CO* adsorbed on Pt, thereby retaining more active sites for H 2 adsorption and oxidation. The HOR exchange current density of Pt/W@NCNF reaches 1.35 times that of commercial Pt/C, and the limiting current density decreases by only 3.4% after introducing 1000 ppm CO in H 2 . Notably, the Pt/W@NCNF-based PEMFCs deliver markedly superior performance across a range of CO concentrations. The present study demonstrates that electronic modulation of Pt is an effective strategy for simultaneously achieving resistance to CO and promoted HOR activity.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
Science Bulletin
·
2025
·
IF 21.1
Tongtong Yang,Heng Liu,Hengjie Liu,Weiyi Zhao,Jiawei Ge,Wenhui Wang,Shuai Yang,Meijian Tang,Kai Wei,Kangcheng Wang,Zeming Qi,Xian Wang,Hao Li,Junjie Ge
Single-atom catalysts (SACs) challenge conventional multi-site catalysis by enabling oxidative processes like H 2 and CO oxidation. However, we herein present that the completely isolated SACs are inactive, while spatially adjacent single-atom pairs (interatomic distance < 4 Å) work cooperatively as the true active sites. Rh atomic densities were precisely tuned between 0.1 wt%–17.5 wt% via graphene quantum dots confinement. Mathematical modeling quantifies the scaling of active pairs versus electrochemical performance, rationalizing activity dependence on atomic proximity. 18 O isotope labeling and in situ synchrotron infrared spectroscopy analyses identified a new reaction mechanism, with water bifunctional dissociation enabled on sub-4 Å Rh pairs, and acts as the rate-determining step towards both CO and H 2 oxidation. While H 2 O enters the COOR process as a reactant and enters the HOR process as a molecular catalyst. Our findings redefine bifunctional catalysis, merging single-atom precision with nanoparticle-like cooperativity for efficient energy conversion systems.
研究领域:
材料科学
·
催化
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电化学
·
能量转换
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）