INORGANIC CHEMISTRY
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2022
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IF 5.436
Hu Yang,Aichuang Zhang,Yunfei Bai,Mingyu Chu,Han Li,Yuan Liu,Peng Zhu,Xiaolei Chen,Chengwei Deng,Xiaolei Yuan
Even though extensive efforts have been devoted to mixing Pd nanocrystals with Ni(OH)2 for the enhanced synergy, it remains a great challenge to incorporate nanosized Ni(OH)2 species on the Pd electrode and reveal their synergy. Herein, we present spongelike Pd nanocrystals with the modification of amorphous Ni(OH)2 species. The catalyst configuration is first considered by compositing Pd with Ni(OH)2 species to optimize the Pd–Pd interatomic distance and then constructing a strongly coupled interface between Pd nanostructures and Ni(OH)2 species. For the ethanol oxidation reaction (EOR) and the formic acid oxidation reaction (FAOR), Pd-Ni(OH)2 composites exhibit an impressive mass activity of 4.98 and 2.65 A mgPd–1, respectively. Most impressively, there is no significant decrease in the EOR activity during five consecutive cycles (50 000 s). A series of CO-poisoning tests have proved that the enhanced EOR and FAOR performances involve synergy between Pd nanostructures and Ni(OH)2 species.
研究领域:
催化
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材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Feiyan Si,Shuai Wang,Yanao Zhang,Ruixin Xue,Yipin Lv,Guozhu Chen,Daowei Gao
Addressing the pivotal challenge of lattice distortion and electronic structure modulation in High-Entropy Alloys (HEAs) for electrochemical catalysis, this investigation presents the synthesis of a novel PtRhNiCoFeGaW HEA in a three-dimensional nanoflower configuration. This design strategically combines enhanced morphological features and a synergistic metallic interaction, propelling the catalytic efficiency forward in methanol and formic acid oxidation reactions (MOR and FAOR). The synthesized HEA nanoflowers exhibit superior mass and specific activities of up to 1.34 mA μg Pt −1 and 4.43 mA cm −2 for MOR, alongside 0.52 mA μg Pt −1 and 1.74 mA cm −2 for FAOR , markedly surpassing those of conventional Pt/C and PtRhNi NFs. This leap in performance is primarily attributed to the intricate elemental synergy within the HEAs, which effectively minimizes CO poisoning (a notorious catalyst deactivator) by improving CO* resistance. Furthermore, the study delineates how the unique nanoflower morphology contributes to exposing a plethora of active sites, thereby maximizing catalytic action. This research not only navigates through the complexities of crafting multi-elemental catalytic systems but also establishes a foundational strategy for developing next-generation HEA-based electrocatalysts, poised to significantly impact future advancements in energy conversion technologies.
研究领域:
材料科学
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电化学
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催化
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of the American Chemical Society
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2023
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IF 15
Chengyuan Dong,Xinyao Wang,Zhipeng Zhu,Changhong Zhan,Xin Lin,Lingzheng Bu,Jinyu Ye,Yucheng Wang,Wei Liu,Xiaoqing Huang
Designing efficient formic acid oxidation reaction (FAOR) catalysts with remarkable membrane electrode assembly (MEA) performance in a direct formic acid fuel cell (DFAFC) medium is significant yet challenging. Herein, we report that the monoclinic-phased platinum–tellurium nanotrepang (m-PtTe NT) can be adopted as a highly active, selective, and stable FAOR catalyst with a desirable direct reaction pathway. The m-PtTe NT exhibits the high specific and mass activities of 6.78 mA cm–2 and 3.2 A mgPt–1, respectively, which are 35.7/22.9, 2.8/2.6, and 3.9/2.9 times higher than those of commercial Pt/C, rhombohedral-phased Pt2Te3 NT (r-Pt2Te3 NT), and trigonal-phased PtTe2 NT (t-PtTe2 NT), respectively. Simultaneously, the highest reaction tendency for the direct FAOR pathway and the best tolerance to poisonous CO intermediate can also be realized by m-PtTe NT. More importantly, even in a single-cell medium, the m-PtTe NT can display a much higher MEA power density (171.4 mW cm–2) and stability (53.2% voltage loss after 5660 s) than those of commercial Pt/C, demonstrating the great potential in operating DFAFC device. The in-situ Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy jointly demonstrate that the unique nanostructure of m-PtTe NT can effectively optimize dehydrogenation steps and inhibit the CO intermediate adsorption, as well as promote the oxidation of noxious CO intermediate, thus achieving the great improvement of FAOR activity, poisoning tolerance, and stability. Density functional theory calculations further reveal that the direct pathway is the most favorable on m-PtTe NT than r-Pt2Te3 NT and t-PtTe2 NT. The higher activation energy to produce CO and the relatively weaker binding with CO of m-PtTe NT result in the better CO tolerance. This work achieves remarkable FAOR and MEA performances of advanced Pt-based anodic catalysts for DFAFCs via a phase engineering strategy.
研究领域:
材料科学
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电化学
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催化
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燃料电池技术
✓ 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）