JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
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
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Chemistry
·
2023
·
IF 13.1
Feng Zhou,Xiaofeng Ke,Yihuang Chen,Mei Zhao,Yun Yang,Youqing Dong,Chao Zou,Xi'an Chen,Huile Jin,Lijie Zhang,Shun Wang
The scarcity, high cost and susceptibility to CO of Platinum severely restrict its application in alkaline hydrogen oxidation reaction (HOR). Hybridizing Pt with other transition metals provides an effective strategy to modulate its catalytic HOR performance, but at the cost of mass activity due to the coverage of modifiers on Pt surface. Herein, we constructed dual junctions’ Pt/nitrogen-doped carbon (Pt/NC) and δ-MoC/NC to modify electronic structure of Pt via interfacial electron transfer to acquire Pt-MoC@NC catalyst with electron-deficient Pt nanoparticles, simultaneously endowing it with high mass activity and durability of alkaline HOR. Moreover, the unique structure of Pt-MoC@NC endows Pt with a high CO-tolerance at 1,000 ppm CO/H 2 , a quality that commercial Pt-C catalyst lacks. The theoretical calculations not only confirm the diffusion of electrons from Pt/NC to MoC/NC could occur, but also demonstrate the negative shift of Pt d -band center for the optimized binding energies of *H, *OH and CO.
研究领域:
材料科学
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催化化学
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理论计算
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2024
·
IF 10.7
Xu Yu,Han Tian,Ziyi Yu,Fantao Kong,Chang Chen,Ziwei Chang,Jian Huang,Xiangzhi Cui,Jianlin Shi
Hydrogen spillover effect-based active catalyst design is an effective strategy to enhance the hydrogen oxidation reaction (HOR) performance, which, unfortunately, still suffers from the high hydrogen spillover energy barrier. Here, a strategy alloying Ir with Ru is proposed to modulate the electronic structure of Ir to accelerate the H* transfer by a novel Ir–Ru–WO2.72 bridge, thus significantly reducing the hydrogen spillover energy barrier from Ir to WO2.72. The IrRu nanoclusters were deposited on a three-dimensional ordered macroporous WO2.72–C framework, and thus the constructed IrRu–WO2.72–C (1.16 wt% Ir and 1.09 wt% Ru) catalyst exhibits excellent HOR and CO-tolerance performance, rather high cell power density, and especially, 4 times higher mass activity than that of Pt/C. The modulation of Ru largely decreases the work function difference between the IrRu clusters and substrate, resulting in a reduced hydrogen spillover barrier via the Ir–Ru–WO2.72 bridge, weakened CO adsorption and fast removal of the adsorbed CO.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Na Ye,Zhao Jiang,Tao Fang
The low-palladium Pd/TaN–C catalyst is synthesized by a surfactant-free solvothermal approach and exhibits high activity (2613.18 mA mg Pd −1 ), durability and CO tolerance for MOR (methanol oxidation reaction) in alkaline media , 12.4 folds that of the commercial Pd/C. XPS and electrochemical results indicate that the interfacial Pd–TaNO bond is generated. This also brings the enhancement of OH ad adsorption responsible for anti-CO poisoning ability. Density Functional Theory (DFT) calculations indicate that the reaction pathway and the rate-determining step are changed for methanol decomposition to CO on the Pd 4 /TaN(001) surface compared with Pd (111). The preferred pathway can be described as: CH 3 OH→CH 3 O→CH 2 O→CHO→CO. Furthermore, the results indicate that the adsorption of OH is enhanced and the energy barrier of COOH formation from CO + OH is reduced with the high concentration of hydroxyl on the Pd 4 /TaN(001) surface, further confirming the bi-functional effect of hydroxyl on the CO tolerance.
研究领域:
电化学
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催化材料
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理论计算
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jiwen Lin,Zhongyao Zhang,Jiaye Qiu,Yujie Wu,Jun Yu,Yongliang Li,Xiangzhong Ren,Lei Zhang,Zhongxin Song
Pt-based catalysts are widely used in hydrogen oxidation reaction (HOR) for the anode of proton exchange membrane fuel cells (PEMFCs). However, high Pt loading and CO poisoning increase the overall cost and stringent requirements for fuel purity. Here, decreasing Pt usage while achieving high anode performance by anchoring Ni single atoms under or adjacent to Pt nanoclusters is studied. The electron interaction between oxophilic Ni single atoms and Pt nanoclusters is beneficial for optimizing the electrocatalytic HOR. The Pt-Ni SA /CNT-2.6 (CNT-carbon nanotube) catalyst with 2.6 wt% low Pt loading shows superior catalytic activity for the HOR, long-time stability, and good CO-tolerant performance in the liquid half-cell and fuel cell of membrane electrode assembly (MEA). Theoretical calculations reveal that the synergy between single atoms and nanoclusters optimizes the d band of Pt and decreases the activation barrier for HOR and CO stripping, thereby enhancing HOR activity and high CO tolerance in PEMFC anodes with a low Pt loading. This work provides a novel design of electron interactions between single atoms and Pt nanoclusters, showing a significant advantage in promoting low-Pt PEMFCs with high power and CO tolerance.
研究领域:
材料科学
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电化学
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燃料电池
✓ 已验证
产品关联
DOI
高影响因子
ACS Omega
·
2022
·
IF 4.132
Jialu Huang,Zhiming Ni,Xiaofan Song,Han Li,Xiaolei Chen,Aichuang Zhang,Hu Yang,Yuan Liu,Peng Zhu,Ping Hua,Xiaolei Yuan
PdPb nanocrystals have drawn considerable attention due to their excellent catalytic properties, while their practical applications have been impeded by the severe degradation of activity, which is caused by the adsorption of intermediates (especially CO) during the operation. Herein, we first present porous PdPb alloys with the incorporation of amorphous Pb(OH)2 species as highly active and stable electrocatalysts. Alloying Pd with Pb species is initially proposed to optimize the Pd–Pd interatomic distance and adjust the d-band center of Pd. Importantly, the amorphous Pb(OH)2 species are beneficial to promoting the formation of OHad and the removal of COad. Therefore, PdPb-Pb(OH)2 catalysts show a mass activity of 3.18 A mgPd–1 and keep excellent stability for the ethanol oxidation reaction (EOR). In addition, further CO stripping and a series of CO poisoning experiments indicate that PdPb-Pb(OH)2 composites possess much better CO tolerance benefiting from the tuned electronic structure of Pd and surface incorporation of Pb(OH)2 species.
研究领域:
材料科学
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电化学
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催化
✓ 已验证
DOI
高影响因子
FARADAY DISCUSSIONS
·
2021
·Vol. 233
·232-243
·
IF 4.008
Pengfei Yao,Jing Cao,Mingbo Ruan,Ping Song,Xue Gong,Ce Han,Weilin Xu
Achieving a highly efficient and durable methanol electro-oxidation catalyst in acid media is critical for the practical utilization of direct methanol fuel cells (DMFCs) at the commercial scale. Herein, we report a facile and effective one-pot strategy for the synthesis of carbon-supported PtCu alloy nanoparticles (PtCu NPs) with a Pt-rich surface, small particle size and uniform dispersion. The as-prepared PtCu NPs with the optimal alloy composition (Pt2Cu) exhibit a significantly improved electrochemical methanol oxidation reaction performance in terms of a high activity, superior CO tolerance and remarkable durability, in contrast to those of commercial Pt/C catalysts in acid media. Particularly, the Pt2Cu/C catalyst exerts a 4.5 times enhancement in the mass activity and a larger If/Ib value compared to those of commercial Pt/C (Pt/Ccomm). The enhanced catalytic activities can be ascribed to the high utilization of Pt and the high index facets of the surface. Also, the addition of Cu downshifts the d-band center of Pt and improves the CO tolerance during the methanol oxidation reaction process. This work provides an efficient strategy for designing desired Pt-based alloys for various catalytic reactions.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2024
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IF 5.5
Xinyi Hu,Hui Xiong,Jiale Dou,Zhao Jiang
It is critical to create the anodic catalysts with high efficiency and economy for direct methanol fuel cells (DMFCs). Here, a series of PtNi/NbN-C catalysts (M=Co, Sn, Ni) are developed using the glycol solvothermal process, to investigate the catalytic effficiency for alkaline methanol oxidation reaction (MOR). Catalytic performance evaluation experiments show that the doped Ni species bring the enhancement effect on Pt/NbN-C for the alkaline MOR. The mass activities of Pt x Ni y /NbN-C show a volcanic trend with the increased Ni contents. PtNi/NbN-C has the highest mass activity (6025.5 mA·mg -1 Pt ) for alkaline MOR, 18.3 times greater than that of the Pt/C commercial catalyst. The LSV, EIS, Tafel, CA and CO stripping results imply PtNi/NbN-C also exhibits the lowest onset potential, charge transfer resistance, fastest kinetics, highest CO tolerance and stability. When the XRD, HRTEM, and XPS analysis are combined, it is discovered that the electronic effect between the Pt, Ni, and NbN species is mostly responsible for the catalytic performance enhancement is mainly depend on the electronic effect among the Pt, Ni and NbN species. The presence of Pt in an electron-deficient state can enhance the conversion of adsorbed methanol and intermediates, evidenced by a direct relationship between the d -band centers and the mass activities for MOR of different catalysts. This study may provide guidance for the development of anodic materials for DMFCs.
研究领域:
材料科学
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催化化学
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燃料电池研究
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2025
·
IF 5.5
Yu Hao,Dongfang Chen,Dongyi Pu,Song Hu,Pavese Doague Nguela,Pucheng Pei,Xiaoming Xu
The development of efficient and durable hydrogen evolution reaction (HER) electrocatalysts is critical for sustainable energy conversion. Although platinum (Pt) serves as a benchmark HER catalyst, its practical application is hindered by the high cost, limited durability, and susceptibility to CO poisoning. In this work, we report a heterojunction Pt-based catalyst, Pt@NCL-MXene, synthesized by LiF etching of MXene and subsequent NH3 calcination. This process introduces dual nitrogen (N) and fluorine (F) doping and yields a nitrogen-doped carbon layer (NCL) coating on Pt nanoparticles with an average size of only 3.4 nm. Compared with conventional Pt–C catalysts, Pt@NCL-MXene exhibits a larger specific surface area, enhanced electron transfer efficiency, and an optimized d-band center, thereby facilitating both H* adsorption and desorption. As a result, Pt@NCL-MXene achieves a significantly lower overpotential of 73 mV at a current density of 100 mA cm–2, alongside improved kinetics and stability under operational conditions. Furthermore, the 9 wt % F-rich MXene support effectively suppresses CO adsorption on Pt, reducing the CO uptake to 0.224 mmol g–1, which is purportedly lower than that of Pt–C (0.264 mmol g–1), thereby mitigating CO poisoning and prolonging the catalyst’s service life. These findings offer insights into the rational design of advanced CO-resistant Pt-based HER electrocatalysts.
研究领域:
材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2020
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IF 5.578
Hau Quoc Pham,Tai Thien Huynh,Son Truong Nguyen,Nam Nguyen Dang,Long Giang Bach,Van Thi Thanh Ho
Direct alcohol fuel cells (DAFCs) use liquid and renewable fuels that have been sparked significant interest in a variety of applications; however, the poor catalytic performance of the state-of-the-art Pt nanoparticles (NPs) over carbon support is a major challenge for further DAFC utilization. Herein, the 1D-bimetallic Pt 3 Co nanowires with a diameter of ~4 nm and the lengths of up to several tens nanometers were grown firstly on the non-carbon Ti 0.7 W 0.3 O 2 nanoparticles via a template- and surfactant-free chemical reduction preparation at room temperature. Electrochemical results indicated that the bimetallic Pt 3 Co NWs/Ti 0.7 W 0.3 O 2 catalyst was an effective electrocatalyst toward alcohol (methanol, ethanol) electrochemical oxidation. For instance, the bimetallic Pt 3 Co NWs/Ti 0.7 W 0.3 O 2 catalyst exhibited high mass activity (MOR of ~393.29 mA m g P t - 1 and EOR of ~341.76 mA m g P t - 1 ), low onset potential (~0.01 V vs. NHE for MOR and ~0.20 V vs. NHE for EOR) and superior CO-tolerance (I f /I b value for MOR of ~3.11 and EOR of ~1.54) in comparison with the conventional carbon-supported Pt nanoparticles (NPs) catalyst. Additionally, the mass activity loss of the Ti 0.7 W 0.3 O 2 -supported Pt 3 Co (NWs) catalyst was ~10.68% of the initial mass activity, which ~4.18-time lower than that of the carbon-supported Pt (NPs) catalyst (~44.66% of the initial mass activity) after 5000 cycles test, indicating the superior stability retention of the as-obtained Pt 3 Co NWs/Ti 0.7 W 0.3 O 2 electrocatalyst . These enhancements were attributable to the combination of the advantageous 1D nanostructures with the internal effect of the Pt 3 Co nanowires, the synergistic effect between Pt-M alloy and TiO 2 -based nanomaterials and the superior anti-corrosion possibility of the non-carbon support.
研究领域:
材料科学
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电化学
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能源科学
✓ 已验证
DOI
高影响因子
ChemCatChem
·
2023
·Vol. 15
·期 10
·e202300255
·
IF 4.5
Quan Zhang,Yuhua Xie,Xia Zhang,Mengxiao Zhao,Qian Chen,Yiman Wu,Jiangfeng Yu,Qiyun Pan,Fangqi Yang,Huihui Lin
Graphical A metal doped strategy was developed via a facile one-step solvent reduction approach, for reducing Pt, Ru and Pd metal ions supported on carbon nanotubes and preparing ternary metal alloy nanoparticles supported on carbon nanotubes (CNTs) electrocatalyst (PtRuPd@CNT). Such a PtRuPd@CNT ternary-alloy catalyst exhibits a superior concentrated methanol oxidation reaction performance including catalytic activity, stability and CO-tolerance. Due to the complex reaction process involving six-electron transfer, high overpotential and slow kinetic rate of methanol oxidation, the development process of direct methanol fuel cells (DMFC) has been hampered. Herein, a simple one-step solvent reduction approach was employed to simultaneously reduce metal ions supported on carbon nanotubes and prepared ternary metal alloy nanoparticles supported on carbon nanotubes electrocatalyst (PtRuPd@CNT). Compared with PtRu@CNT binary metal catalyst, the as-prepared PtRuPd@CNT ternary metal catalyst displayed more outstanding methanol oxidation reaction (MOR) catalytic performance and good CO anti-poisoning ability. In the case of using 8 M methanol, the MOR performance of PtRuPd@CNT was 1.8 times better than the PtRu@CNT electrocatalyst. The addition of the Pd atom regulates the surface electronic structure of PtRu alloy, and the strong electronic interaction enhances the MOR activity of the PtRu@CNT catalyst. Furthermore, the addition of the Pd atom in the PtRuPd@CNT electrocatalyst also diminishes adsorption of CO intermediate species on the Pt surface, boosting the CO anti-poisoning ability of the catalyst and improving the stability. Therefore, the PtRuPd@CNT electrocatalyst incorporating the Pd atoms could actualize the practical application prospect as an efficient concentrated DMFC anode catalyst.
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
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yafeng Wang,Xian Luo,Wenjie Lu,Bin Huang,Yanqing Yang
Since Pt- and Pd-based catalysts, as the most common anode catalysts, usually suffer from CO poisoning issue during the electro oxidation of ethylene glycol, it is essential to explore more high-efficiency Pt- and Pd-free ethylene glycol oxidation reaction (EGOR) catalysts for better service in direct ethylene glycol fuel cells (DEGFCs). In this work, RhCo alloyed nanodendritic catalysts applied on EGOR in alkaline solution are designed and synthesized by a solvothermal method. The RhCo nanodendrites consist of radially distributed pine tree shaped flakes and rod-like crystals. The mass activity for the as-prepared Rh 3 Co 1 nanodendrites during the EGOR reaches up to 3018.7 mA mg −1 , which is 2.2-folds higher than that of commercial Pt/C. Moreover, the Rh 3 Co 1 nanodendrites exhibit better stability and CO tolerance toward the EGOR than pure Rh nanodendrites and commercial Pt/C. Experimental observations in combination with density functional theory (DFT) calculations reveal that the notably promoted catalytic performances of Rh 3 Co 1 nanodendrites are mainly attributed to the distinct nanodendritic morphology and the synergistic effect of Rh and Co. This work provides a valuable insight for developing efficient electrocatalysts for DEGFCs.
研究领域:
材料科学
·
电化学
✓ 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）