APPLIED SURFACE SCIENCE
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2020
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IF 6.182
Mengran Lou,Ruiying Wang,Lili Yang,Dianzeng Jia,Zhipeng Sun,Luxiang Wang,Yong Guo,Xingchao Wang,Jie Zhang,Hongli Shi
Direct formic acid fuel cells have great application potential in the energy field, but their commercialization is hindered by the CO poisoning and low performance of Pd-based anode catalysts. In this study, novel composite catalysts composed of Pd, organic-inorganic hybrid imidazole ionic liquid polyoxometalates, and N,P-codoped coal-based carbon fibers with good dispersion and smaller Pd nanoparticles were synthesized successfully. Physical and electrochemical characterizations revealed that the as-prepared Pd-based composite catalysts have excellent CO poisoning resistance and enhanced electrocatalytic activity in formic acid electrooxidation. Notably, the CO oxidation onset potential of a catalyst modified by imidazole ionic liquid polyoxometalate with long alkyl chain was 0.1 V lower than that of the unmodified catalyst. The mass activity of the as-prepared Pd catalyst in formic acid oxidation was 754.1 mA mg −1 Pd . It is expected that organic-inorganic hybrid polyoxometalates can be further applied to fuel cell catalysts.
研究领域:
材料科学
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电化学
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能源技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
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2024
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IF 5.4
Tao Chen,Manli Wang,Donghang Hu,Qianlin Ju,Kaige Zhao,Liang Fu,Zelin Chen,Xiaolong Yu,Changjiu Li
The mainstream electrocatalysts for direct ethanol fuel cells (DEFCs) are Pt- or Pd-based nanomaterials, which are severely hampered by CO intermediate poisoning and the relatively low selectivity of the C1 pathway in anodic ethanol oxidation reaction (EOR), thereby impeding the efficiency enhancement and practical application of DEFCs. Herein, we report a Pt-decorated amorphous PdS nanowire [denoted as a-Pd(S)NWs/Pt] catalyst with abundant crystalline/amorphous heterogeneous interfacial active sites for alkaline EOR. The a-Pd(S)NWs/Pt was demonstrated a superior EOR mass activity of 6.16 A·mgPd+Pt–1, which is 22.81 times over that of commercial Pt/C (0.27 A·mgPt–1) and 34.22 times over that of commercial Pd/C (0.18 A·mgPd–1). Additionally, the a-Pd(S)NWs/Pt exhibited considerable stability, significantly enhanced resistance to CO poisoning and enhanced selectivity for the EOR C1 pathway. Density functional theory calculations and experimental results further revealed that the optimized COads and OHads binding energies due to the decoration of Pt nanoclusters can be responsible for the enhanced CO resistance and C1 selectivity of a-Pd(S)NWs/Pt. Furthermore, benefiting from its optimized electronic configuration at the interfacial active sites and the appropriate intermediate adsorption capacity, the a-Pd(S)NWs/Pt electrocatalyst was successfully extended to the electrocatalytic methanol and ethylene glycol oxidation reaction systems.
研究领域:
材料科学
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电化学
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催化
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2024
·Vol. 48
·期 17
·7964-7971
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IF 2.7
Xuanhua Zhang,Chao Wang,Chao Luan,Mengyin Liao,Wenyuan Xu
Direct methanol fuel cells (DMFC) are a promising new energy source. However, the lack of high-performance and low-cost methanol oxidation electrocatalysts hinders their commercial application. Firstly, we successfully prepared NENU-5-derived molybdenum carbide material (Cu-MoC) via a co-precipitation and high-temperature carbonization method using a material composed of a copper-based metal–organic skeleton and a molybdenum-based carbide as the main body. Secondly, PtCu nano-alloy catalysts (Pt/Cu-MoC) were prepared using a unique, spontaneous single replacement reaction after metal–organic skeleton (MOF) carbonization. Through the synergistic effect between Pt and Cu and the strong interaction between Mo2C and PtCu, the electronic structure of the Pt is modified, the energy of the d-band center is reduced, electron exchange is accelerated, and catalytic activity is enhanced. Compared with a commercial Pt/C catalyst in alkaline environments, the Pt0.10/Cu-MoC catalyst has a better MOR catalytic activity (563.25 mA mgPt−1), which is 1.5 times higher than that of commercial Pt/C (376.67 mA mgPt−1). The Pt0.10/Cu-MoC catalyst has an onset potential for CO oxidation that is 16 mV lower than that of commercial Pt/C, indicating better resistance to CO poisoning. Exploring carbon materials derived from MOFs with excellent junction support and using them as carriers to prepare Pt-based catalysts is a practical and feasible approach. It provides a way to develop new Pt-based catalysts that perform efficient MOR.
研究领域:
材料科学
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电化学
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催化作用
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2024
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IF 18.5
Xiaoning Wang,Xiaochun Gao,Li Tang,Puhua Sun,Ying Liu,Shaoqi Hou,Yanfu Tong,Xitao Yin,Xiaoguang Ma
The challenges encountered by Pt-based electrocatalysts in alkaline hydrogen oxidation reaction include high Pt dosage and conflicting demands for modulating adsorption strengths among diverse intermediates. Here, an ultrasmall Pt cluster grafted on antimony tin oxide nanocrystalline with strong electron donor ability to minimal Pt dosage yet maximized electrocatalytic performance is developed. Mechanism studies show that the formation of Pt–Sn/Sb interaction at the heterointerface and the resultant reversed electron transfer selectively enhance the adsorption for OH - while concurrently weakening the binding strength for *H and CO toward Pt clusters. This accelerates the kinetics of H 2 /CO oxidation by promoting the binding of OH species with *H/*CO, yielding the catalyst with up to 5.7-fold higher mass-specific activity than benchmark Pt/C and increased resistance to CO poisoning. This work demonstrates the rational design of the synergistic multi-site interactions towards advanced Pt-based catalysts.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
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