ACS Catalysis
·
2024
·
IF 11.3
Chaoyi Yang,Guangqin Wang,Jianchao Yue,Zihao Dai,Wei Luo
The development of active and anti-CO-poisoning Pt-based electrocatalysts toward an alkaline hydrogen oxidation reaction (HOR) is highly desirable for the practical application of anion exchange membrane fuel cells. Herein, we report the synthesis of intermetallic Pt alloys with introduction of oxophilic Sn (including Pt3Sn and PtSn), significantly boosting the alkaline HOR performance and CO tolerance. Experimental results including in situ surface-enhanced infrared absorption spectroscopy and theoretical calculations unravel that the d band centers of Pt in Pt3Sn and PtSn are notably down shift due to the introduction of oxophilic Sn, thereby leading to the decreased adsorption energy of both hydrogen and CO, which together with the enhanced adsorption energy of OH species on Sn sites contribute the lowered energy barrier for water formation and CO oxidation. As expected, the obtained Pt3Sn and PtSn both present improved HOR performance and anti-CO-poisoning ability. Specially, Pt3Sn depicts three times specific activity and four times mass activity higher than that of Pt, while PtSn maintains over 90% HOR activity after the CO poisoning.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yunjie Zhou,Feiyang Yu,Zhongling Lang,Haodong Nie,Zhenzhen Wang,Mingwang Shao,Yang Liu,Huaqiao Tan,Yangguang Li,Zhenhui Kang
Platinum (Pt) is practical available candidate for satisfying the requirements of anode catalysts in the proton exchange membrane fuel cells (PEMFCs). Totally dispersed Pt is an ideal way to minimize Pt use, and the develop of Pt-single-atom based hydrogen oxidation reaction (HOR) catalysts should be carried out in a multi-component/-function model system with a clear active site (Pt-single-atom) geometric structure. This work combines the well-defined Na 6 [H 2 PtW 6 O 24 ] clusters and multi-function carbon dots (CDs) to show the highly efficient Pt-single-atom catalyst design for HOR in acid. The mass activity and exchange current density of POMs/CDs (2.18 wt% Pt) achieved 86.72 A mg pt −1 and 3.78 A mg pt −1 , respectively, which were 9.5 and 14 times that of 20% Pt/C. Also, this catalyst exhibits better performance than 20% Pt/C in the test of single cell, including higher open circuit potential (OCP), higher power density and better long-time stability. In particular, CDs can effectively improve the catalytic performance of POMs by enhancing the electron acquisition ability of Pt in POMs, the conductivity of composites, the structure stability, the ability to resist toxicity and accelerating the transfer of H + produced on POMs.
研究领域:
材料科学
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能源化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2025
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IF 5.5
Na Jin,Xiao Yang,Yong Li,Wanjing Lai,Hailin Jiang,Yanghua Li,Kuo Liu,Yimeng Cai,Linjie Zhang,Lili Han
Hydrogen, characterized by its high energy density, efficiency, and environmentally benign output, emerges as a promising alternative to fossil fuels. However, the development of robust hydrogen oxidation reaction (HOR) catalysts for efficient energy conversion remains a significant challenge. Herein, a NiRu nanoalloy catalyst supported on N-doped hollow carbon nanocages (NiRu/NC) is synthesized via a tandem pyrolysis method. The NiRu/NC catalyst exhibits superior alkaline HOR activity, achieving diffusion-limited current density of 2.56 mA cm–2 and maintaining stability for 80,000 s with a decay rate of only 5.9%, compared to a 28.7% decay rate for benchmark Pt/C after 35,000 s. Additionally, it demonstrates remarkable resistance to CO poisoning, with the current density decreasing by only 50.7% after 1800 s, while the current density of Pt/C dropped to 0 after 800 s. Density functional theory calculations indicate that Ni in the NiRu nanoalloy effectively modulates the electron distribution, thereby ameliorating the electronic structure and enhancing the adsorption of reaction intermediates. These optimizations endow NiRu/NC with both favorable hydrogen-binding energy (HBE) and hydroxyl-binding energy (OHBE), leading to improved HOR efficiency. This work not only offers an innovative approach for synthesizing high-performance alloy-based HOR catalysts but also deepens the fundamental understanding of the bimetallic synergistic mechanisms in HOR catalysis.
研究领域:
材料科学
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电催化
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能源转换
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
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
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Wanli Liang,Zhichen Le,Pengyu Dong,Zixuan Dan,Jiaxuan Chen,Hao Zhang,Jian Chen,Fangyan Xie,Nan Wang,Yanshuo Jin,Hui Meng
The development of hydrogen energy is limited by the high cost of platinum group metals (PGM). There is an urgent need to design efficient PGM-free electrocatalysts in the hydrogen electrode. Herein, Janus Ni/W bimetallic materials are proposed as an effective PGM-free bifunctional hydrogen electrocatalyst. By constructing the bimetallic materials, a synergistic effect is realized to enhance the reaction kinetics and improve the catalytic performance. In general, Ni can provide excellent H ad sites, and W serves as OH ad sites. Therefore, the synergistic effect of Ni and W can improve the kinetics of hydrogen evolution reaction and the hydroxide oxidation reaction. Ni/W@NF can obtain the hydrogen evolution reaction current density of 10 mA cm −2 with an overpotential of only 62.6 mV, and the exchange current density of hydroxide oxidation reaction can reach 1.83 mA cm −2 . This work provides a new idea for the design of high-efficiency and low-cost PGM-free bifunctional hydrogen electrocatalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2019
·Vol. 6
·期 10
·2900-2905
·
IF 5.934
Chang Long,Kun Wang,Yanan Shi,Zhongjie Yang,Xiaofei Zhang,Yin Zhang,Jianyu Han,Yini Bao,Lin Chang,Shaoqin Liu,Zhiyong Tang
Optimization of the hydrogen binding energy by controlling the surface electronic structure of electrocatalysts is of great significance in the hydrogen oxidation reaction (HOR) in alkaline electrolytes. Herein, we demonstrated that the surface electronic structure of PtRu bimetallic nanoparticles could be finely tuned through the alloying degree; this led to enhanced HOR performance in an alkaline solution. The optimized Pt0.65Ru0.35 with high alloying degree exhibited the exchange current density of 4.16 A m−2, which was about 1.5 and 2.2 times those of Pt0.74Ru0.26 with a low alloying degree (2.75 A m−2) and Pt/C (1.89 A m−2), respectively.
研究领域:
化学
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材料科学
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电催化
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2023
·
IF 2.8
Zhang Chao,Zhang Zhengping,Niu Jin,Li Zhilin,Wang Feng
Platinum catalysts with {111} surface has obvious advantages, but the control of {111} exposure usually requires surfactants which cover the surface and decrease the catalytic performance. In this paper, tetrahedral platinum nanoparticle catalysts were successfully prepared with a simple one-step hydrothermal method and their size were successfully controlled under sub-5 nm. The tetrahedral morphology was controlled through the decomposition of dimethylamine by DMF and the small size was determined by alcohol acid radical. Because of the profitable effect of the amines for the tetrahedral morphology, no surfactant was need during the preparation. The catalysis activity was assured by the tetrahedral morphology with Pt {111} exposure without the surfactant covering, and the small size further increased the number of activity sites. For HOR, the catalyst showed higher activity, stronger anti-CO poisoning performance and longer stability than those of commercial catalyst with the same platinum load. For ORR, the catalyst also showed better performances which further promoted the four-electron reaction. Our simple preparation method successfully achieved the aims of the morphology control, size control and the elimination of surfactant, which effectively assured the good catalyst performances. The simple preparation path of such good catalysts shows a great application potential. Graphical Abstract
研究领域:
材料科学
·
电催化
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Xuzhao Shi,Wei Song,Tao Wei,Kui Zhang,Zhigang Shao
The anode Pt catalyst of a proton-exchange membrane fuel cell (PEMFC) is susceptible to poisoning by trace amounts of CO in hydrogen, which restricts its large-scale commercialisation. Therefore, developing PEMFC catalysts with CO tolerance is crucial as it would reduce the requirement for hydrogen purity. In this study, we present a CO-tolerant catalyst for the PEMFC anode synthesised by loading Pt onto a polyaniline-modified conductive carbon composite support (Pt/C-PANI). The results showed that the catalyst containing 5% PANI in the composite support (Pt/C-PANI-5) exhibited optimal hydrogen oxidation reaction activity and CO tolerance. Electrochemical tests showed that the current drop of Pt/C-PANI-5 was 6.8%, compared to 20% and 12% for Pt/C-sys and commercial PtRu/C catalysts, respectively. Furthermore, results of the single-cell test confirmed improved CO tolerance. These findings provide a potential solution for developing cost-effective fuel cell catalysts with improved CO tolerance.
研究领域:
材料科学
·
能源工程
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Yuting Yang,Luyan Shi,Qinrui Liang,Yi Liu,Jiaxin Dong,Tayirjan Taylor Isimjan,Bao Wang,Xiulin Yang
A high-performance and highly CO-resilient hydrogen oxidation reaction (HOR) electrocatalyst is heralded as core material to solve the commercial deployment of hydrogen fuel cells. Phosphorus vacancies, as a type of delicate point defect, could effectively and flexibly modulate the catalytic performance. Therefore, based on the vacancy design philosophy of “less is more”, we synthesize a phosphorus-vacancy-rich Pd 3 P@C (V p -Pd 3 P@C) catalyst with bowl-like hemisphere structure for alkaline HOR, for the first time. The V p -Pd 3 P@C catalyst exhibits remarkable mass activity and exchange current density of 1.66 mA μg Pd –1 and 3.2 mA cm –2 , respectively, surpassing those of Pd 3 P@C (0.45 mA μg Pd –1 , 1.78 mA cm –2 ) and commercial Pt/C (0.3 mA μg Pt –1 , 2.29 mA cm –2 ). Intriguingly, the catalyst can tolerate 1000 ppm CO that Pt/C catalyst lacks. Density functional theory calculations uncover that the optimal local coordination environment and favorable electronic structure that rooted from phosphorus vacancy enable optimum adsorption kinetics of hydrogen and hydroxyl while concomitantly suppressing Pd 4 d → CO 2π* back donation, contributing to the remarkable HOR reactivity and CO tolerance.
研究领域:
材料科学
·
电化学
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能源材料
·
催化
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2020
·
IF 8.247
Jungyeon Ji,Yongjin Chung,Yongchai Kwon
A catalyst capable of high performance and good durability is developed for use in anode of flow-type membraneless hydrogen peroxide fuel cells (HPFCs). For that, cobalt phthalocyanine (CoPc) is immobilized onto reduced graphene oxide (rGO) linked to polyacrylic acid (PAA) surface modifier (rGO/PAA/CoPc). CoPc moiety containing PAA is tightly immobilized due to physical entrapment, axial ligand and stabilization of intermediates. According to evaluations, the amount of CoPc immobilized in rGO/PAA/CoPc is twice than that in rGO/CoPc because rGO and CoPc are weakly connected by π-π conjugation without PAA acting as axial ligand to form coordinate bond with Co core within CoPc. In rGO/PAA/CoPc, current density for hydrogen peroxide oxidation reaction (HPOR) is 2.7 times higher than that measured in rGO/CoPc due to axial ligand role of PAA activating two HPOR pathways, wheras rGO/CoPc is only linked to one HPOR pathway. Even in stability test, rGO/PAA/CoPc preserves 90.0% of its initial HPOR current density, while that of Ni bulk is decreased by 30.6%. When performance of HPFC using rGO/PAA/CoPc is measured with a low concentration of H 2 O 2 (0.1 mol L -1 ) under physiological condition , its maximum power density (72.1 ± 2.68 μWcm −2 ) is better than that of HPFC using rGO/CoPc (38.3 ± 0.20 μWcm −2 ).
研究领域:
化学
·
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2021
·Vol. 12
·期 1
·1-8
·
IF 14.919
Zhan Changhong,Xu Yong,Bu Lingzheng,Zhu Huaze,Feng Yonggang,Yang Tang,Zhang Ying,Yang Zhiqing,Huang Bolong,Shao Qi,Huang Xiaoqing
High-entropy alloys (HEAs) with unique physicochemical properties have attracted tremendous attention in many fields, yet the precise control on dimension and morphology at atomic level remains formidable challenges. Herein, we synthesize unique PtRuNiCoFeMo HEA subnanometer nanowires (SNWs) for alkaline hydrogen oxidation reaction (HOR). The mass and specific activities of HEA SNWs/C reach 6.75 A mg Pt+Ru −1 and 8.96 mA cm −2 , respectively, which are 2.8/2.6, 4.1/2.4, and 19.8/18.7 times higher than those of HEA NPs/C, commercial PtRu/C and Pt/C, respectively. It can even display enhanced resistance to CO poisoning during HOR in the presence of 1000 ppm CO. Density functional theory calculations reveal that the strong interactions between different metal sites in HEA SNWs can greatly regulate the binding strength of proton and hydroxyl, and therefore enhances the HOR activity. This work not only provides a viable synthetic route for the fabrication of Pt-based HEA subnano/nano materials, but also promotes the fundamental researches on catalysis and beyond.
研究领域:
材料科学
·
催化
·
纳米技术
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Sustainable Materials and Technologies
·
2025
·
IF 9.2
Jingyuan Wei,Yanhui Song,Manyuan Gan,Guodong An,Yongqing Shen,Xiaohui Zhao,Yi Zhang,Peizhi Liu,Bingshe Xu,Junjie Guo
Modifying the catalyst's electronic structure is essential for improving the hydrazine oxidation reaction (HzOR) and alkaline hydrogen evolution reaction (HER), but it is still very difficult. We have developed a new heterostructured electrocatalyst in this work using Ru nanosheets and NiCo layered double hydroxides (LDH). In-situ Raman and theoretical studies show that the heterostructure of Ru/NiCo LDH lowers absorption of hydrogen's Gibbs free energy and the d-band center of Ru/NiCo LDH (from −1.7250 to −1.3341 eV), causing the directed development of interfacial H 2 O (ΔG H* , from 1.65 to 0.23 eV). With an overpotential of 19 and 75 mV to achieve 10 and 100 mA cm −2 for HER, these beneficial characteristics provide the Ru/NiCo LDH with exceptional electrocatalytic capabilities. For HzOR, 10 and 100 mA cm −2 may be produced using just −118 and−112 mV, respectively. The Ru/NiCo LDH electrolyzer also only needs 22 and 223 mV to produce 10 and 100 mA cm −2 , respectively. This work lays the groundwork for developing bifunctional catalysts for the green hydrogen industry.
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）