共查询到20条相似文献,搜索用时 5 毫秒
1.
Nanoporous Graphene with Single‐Atom Nickel Dopants: An Efficient and Stable Catalyst for Electrochemical Hydrogen Production 下载免费PDF全文
Dr. H.‐J. Qiu Dr. Yoshikazu Ito Weitao Cong Dr. Yongwen Tan Dr. Pan Liu Dr. Akihiko Hirata Dr. Takeshi Fujita Prof. Zheng Tang Prof. Mingwei Chen 《Angewandte Chemie (International ed. in English)》2015,54(47):14031-14035
Single‐atom nickel dopants anchored to three‐dimensional nanoporous graphene can be used as catalysts of the hydrogen evolution reaction (HER) in acidic solutions. In contrast to conventional nickel‐based catalysts and graphene, this material shows superior HER catalysis with a low overpotential of approximately 50 mV and a Tafel slope of 45 mV dec?1 in 0.5 M H2SO4 solution, together with excellent cycling stability. Experimental and theoretical investigations suggest that the unusual catalytic performance of this catalyst is due to sp–d orbital charge transfer between the Ni dopants and the surrounding carbon atoms. The resultant local structure with empty C–Ni hybrid orbitals is catalytically active and electrochemically stable. 相似文献
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Yu Zhang Weimeng Chi Baiqing Zhang Zhuoxun Yin Xinzhi Ma Yang Zhou Wei Chen Lingling Xu Jinlong Li 《欧洲无机化学杂志》2023,26(34):e202300492
The conventional electrolytic water-splitting process for hydrogen production is plagued by high energy consumption, low efficiency, and the requirement of expensive catalysts. Therefore, finding effective, affordable, and stable catalysts to drive this reaction is urgently needed. We report a nanosheet catalyst composed of carbon nanotubes encapsulated with MoC/Mo2C, the Ni@MoC-700 nanosheet showcases low overpotentials of 275 mV for the oxygen evolution reaction and 173 mV for the hydrogen evolution reaction at a current density of 10 mA ⋅ cm−2. Particularly noteworthy is its outstanding performance in a two-electrode system, where a cell potential of merely 1.64 V is sufficient to achieve the desired current density of 10 mA ⋅ cm−2. Furthermore, the catalyst demonstrates exceptional durability, maintaining its activity over a continuous operation of 40 hours with only minimal attenuation in overpotential. These outstanding activity levels and long-term stability unequivocally highlight the promising potential of the Ni@MoC-700 catalyst for large-scale water-splitting applications. 相似文献
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Molybdenum Phosphosulfide: An Active,Acid‐Stable,Earth‐Abundant Catalyst for the Hydrogen Evolution Reaction 下载免费PDF全文
Dr. Jakob Kibsgaard Prof. Thomas F. Jaramillo 《Angewandte Chemie (International ed. in English)》2014,53(52):14433-14437
Introducing sulfur into the surface of molybdenum phosphide (MoP) produces a molybdenum phosphosulfide (MoP|S) catalyst with superb activity and stability for the hydrogen evolution reaction (HER) in acidic environments. The MoP|S catalyst reported herein exhibits one of the highest HER activities of any non‐noble‐metal electrocatalyst investigated in strong acid, while remaining perfectly stable in accelerated durability testing. Whereas mixed‐metal alloy catalysts are well‐known, MoP|S represents a more uncommon mixed‐anion catalyst where synergistic effects between sulfur and phosphorus produce a high‐surface‐area electrode that is more active than those based on either the pure sulfide or the pure phosphide. The extraordinarily high activity and stability of this catalyst open up avenues to replace platinum in technologies relevant to renewable energies, such as proton exchange membrane (PEM) electrolyzers and solar photoelectrochemical (PEC) water‐splitting cells. 相似文献
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电催化制氢是解决当前能源危机的重要手段之一。 研究高效稳定的非贵金属电催化剂是电催化制氢商业应用的重点。 本文通过直接高温热解双金属沸石咪唑骨架,制备了一种氮掺杂石墨炭(NC)包覆均匀分布的钴纳米颗粒电催化剂(V-Co@NC,这里V是vacancy缩写),前躯体中的Zn元素有效地防止钴纳米颗粒的聚集,并有助于生成均匀分布的钴纳米颗粒。 这种特殊的纳米结构可防止钴与电解液的直接接触,提升了其循环稳定性,同时,氮元素的掺杂提升了导电性,有利于电催化制氢性能的提升。 结果表明,所制备的V-Co@NC催化剂在酸性和碱性电解液中均具有良好的催化性能,且经过5000次循环测试后催化活性基本保持不变,具有良好的应用前景。为高活性和高选择性的电催化制氢催化剂的发展提供一种全新的途径。 相似文献
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Sean T. Hunt Tarit Nimmanwudipong Prof. Yuriy Román‐Leshkov 《Angewandte Chemie (International ed. in English)》2014,53(20):5131-5136
Transition‐metal carbides (TMCs) exhibit catalytic activities similar to platinum group metals (PGMs), yet TMCs are orders of magnitude more abundant and less expensive. However, current TMC synthesis methods lead to sintering, support degradation, and surface impurity deposition, ultimately precluding their wide‐scale use as catalysts. A method is presented for the production of metal‐terminated TMC nanoparticles in the 1–4 nm range with tunable size, composition, and crystal phase. Carbon‐supported tungsten carbide (WC) and molybdenum tungsten carbide (MoxW1?xC) nanoparticles are highly active and stable electrocatalysts. Specifically, activities and capacitances about 100‐fold higher than commercial WC and within an order of magnitude of platinum‐based catalysts are achieved for the hydrogen evolution and methanol electrooxidation reactions. This method opens an attractive avenue to replace PGMs in high energy density applications such as fuel cells and electrolyzers. 相似文献
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MoS2 Nanosheets Supported on 3D Graphene Aerogel as a Highly Efficient Catalyst for Hydrogen Evolution 下载免费PDF全文
Yufei Zhao Xiuqiang Xie Jinqiang Zhang Dr. Hao Liu Hyo‐Jun Ahn Prof. Kening Sun Prof. Guoxiu Wang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(45):15908-15913
The development of efficient catalysts for electrochemical hydrogen evolution is essential for energy conversion technologies. Molybdenum disulfide (MoS2) has emerged as a promising electrocatalyst for hydrogen evolution reaction, and its performance greatly depends on its exposed edge sites and conductivity. Layered MoS2 nanosheets supported on a 3D graphene aerogel network (GA‐MoS2) exhibit significant catalytic activity in hydrogen evolution. The GA‐MoS2 composite displays a unique 3D architecture with large active surface areas, leading to high catalytic performance with low overpotential, high current density, and good stability. 相似文献
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Can Li Dr. Zheng Chen Dr. Hong Yi Yi Cao Dr. Lei Du Dr. Yidong Hu Fanpeng Kong Prof. Dr. Richard Kramer Campen Prof. Dr. Yunzhi Gao Prof. Dr. Chunyu Du Prof. Dr. Geping Yin Prof. Dr. Igor Ying Zhang Dr. Yujin Tong 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(37):16036-16041
The essence of developing a Pt-based single-atom catalyst (SAC) for hydrogen evolution reaction (HER) is the preparation of well-defined and stable single Pt sites with desired electrocatalytic efficacy. Herein, we report a facile approach to generate uniformly dispersed Pt sites with outstanding HER performance via a photochemical reduction method using polyvinylpyrrolidone (PVP) molecules as the key additive to significantly simplify the synthesis and enhance the catalytic performance. The as-prepared catalyst displays remarkable kinetic activities (20 times higher current density than the commercially available Pt/C) with excellent stability (76.3 % of its initial activity after 5000 cycles) for HER. EXAFS measurements and DFT calculations demonstrate a synergetic effect, where the PVP ligands and the support together modulate the electronic structure of the Pt atoms, which optimize the hydrogen adsorption energy, resulting in a considerably improved HER activity. 相似文献
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Can Li Zheng Chen Hong Yi Yi Cao Lei Du Yidong Hu Fanpeng Kong Richard Kramer Campen Yunzhi Gao Chunyu Du Geping Yin Igor Ying Zhang Yujin Tong 《Angewandte Chemie (International ed. in English)》2020,59(37):15902-15907
The essence of developing a Pt‐based single‐atom catalyst (SAC) for hydrogen evolution reaction (HER) is the preparation of well‐defined and stable single Pt sites with desired electrocatalytic efficacy. Herein, we report a facile approach to generate uniformly dispersed Pt sites with outstanding HER performance via a photochemical reduction method using polyvinylpyrrolidone (PVP) molecules as the key additive to significantly simplify the synthesis and enhance the catalytic performance. The as‐prepared catalyst displays remarkable kinetic activities (20 times higher current density than the commercially available Pt/C) with excellent stability (76.3 % of its initial activity after 5000 cycles) for HER. EXAFS measurements and DFT calculations demonstrate a synergetic effect, where the PVP ligands and the support together modulate the electronic structure of the Pt atoms, which optimize the hydrogen adsorption energy, resulting in a considerably improved HER activity. 相似文献
12.
《Angewandte Chemie (International ed. in English)》2017,56(18):4941-4944
The development of technologically viable electrodes for the electrochemical oxygen evolution reaction (OER) is a major bottleneck in chemical energy conversion. This article describes a facile one‐step hydrothermal route to deposit microcrystals of a robust Dexter–Silverton polyoxometalate oxygen evolution catalyst, [Co6.8Ni1.2W12O42(OH)4(H2O)8], on a commercial nickel foam electrode. The electrode shows efficient and sustained electrochemical oxygen evolution at low overpotentials (360 mV at 10 mA cm−2 against RHE, Tafel slope 126 mV dec−1, faradaic efficiency (96±5) %) in alkaline aqueous solution (pH 13). Post‐catalytic analyses show no mechanical or chemical degradation and no physical detachment of the microcrystals. The results provide a blueprint for the stable “wiring” of POM catalysts to commercial metal foam substrates, thus giving access to technologically relevant composite OER electrodes. 相似文献
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石墨烯基催化剂的设计合成与电催化应用 总被引:1,自引:1,他引:1
为了解决能源匮乏和环境污染的问题,研究人员正致力于寻找清洁可持续的新能源。 其中,氧气还原、氧气析出、析氢反应等是紧密联系新型清洁能源获取和存贮的重要电化学反应。 为了提高其能量转化效率,电催化剂(如碳载铂Pt/C)被广泛地用于降低其反应活化能、提高能量转化效率。 近年来,石墨烯作为一种具有高比表面积和优异导电性的二维碳材料受到了广泛关注。 通过表面杂原子掺杂、缺陷调控和引入催化活性组分等方式,获得了催化性能与贵金属催化剂相媲美,且低价格和高稳定性的非贵金属石墨烯基催化材料。 针对氧气还原、氧气析出和析氢反应在燃料电池、金属-空气电池和电催化水分解中的应用,本文概括综述了通过表/界面结构性质调控提高石墨烯电催化性能和稳定性,获得具有双功能或复合催化性能的石墨烯基催化剂的最新研究进展。 最后总结和展望了亟待解决的问题及未来的发展趋势。 相似文献
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Xiangyu Meng Prof. Dr. Chao Ma Luozhen Jiang Prof. Dr. Rui Si Prof. Dr. Xianguang Meng Dr. Yunchuan Tu Prof. Dr. Liang Yu Prof. Dr. Xinhe Bao Prof. Dr. Dehui Deng 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(26):10588-10593
Perturbing the electronic structure of the MoS2 basal plane by confining heteroatoms offers the opportunity to trigger in-plane activity for the hydrogen evolution reaction (HER). The key challenge consists of inducing the optimum HER activity by controlling the type and distribution of confined atoms. A distance synergy of MoS2-confined single-atom rhodium is presented, leading to an ultra-high HER activity at the in-plane S sites adjacent to the rhodium. By optimizing the distance between the confined Rh atoms, an ultra-low overpotential of 67 mV is achieved at a current density of 10 mA cm−2 in acidic solution. Experiments and first-principles calculations demonstrate a unique distance synergy between the confined rhodium atoms in tuning the reactivity of neighboring in-plane S atoms, which presents a volcanic trend with the inter-rhodium distance. This study provides a new strategy to tailor the activity of MoS2 surface via modulating the distance between confined single atoms. 相似文献
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A Molecular Copper Catalyst for Electrochemical Water Reduction with a Large Hydrogen‐Generation Rate Constant in Aqueous Solution 下载免费PDF全文
Peili Zhang Prof. Mei Wang Yong Yang Tianyi Yao Prof. Licheng Sun 《Angewandte Chemie (International ed. in English)》2014,53(50):13803-13807
The copper complex [(bztpen)Cu](BF4)2 (bztpen=N‐benzyl‐N,N′,N′‐tris(pyridin‐2‐ylmethyl)ethylenediamine) displays high catalytic activity for electrochemical proton reduction in acidic aqueous solutions, with a calculated hydrogen‐generation rate constant (kobs) of over 10000 s?1. A turnover frequency (TOF) of 7000 h?1 cm?2 and a Faradaic efficiency of 96 % were obtained from a controlled potential electrolysis (CPE) experiment with [(bztpen)Cu]2+ in pH 2.5 buffer solution at ?0.90 V versus the standard hydrogen electrode (SHE) over two hours using a glassy carbon electrode. A mechanism involving two proton‐coupled reduction steps was proposed for the dihydrogen generation reaction catalyzed by [(bztpen)Cu]2+. 相似文献
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Graphdiyne(GDY),which is composed of sp2-/sp-hybridized carbon atoms,has attracted increasing attention.In the structure of GDY,the existence of large triangular-like pores,well dispersed electron-rich cavities as well as a large π-conjugated structure endows GDY with a natural bandgap,fast electron/ion transport,and tunable electronic properties.These unique features make GDY competitive in areas of gas separation and capture,electronics,detectors,catalysts,biomedicine and therapy,and energy-related fields.Benefiting from the facile synthesis method,various GDY structures and GDY-based composites have been successfully prepared and show great potential in the practical application of energy storage and catalysis areas.Here,this review aims at providing a timely and comprehensive update on the preparation and application of GDY materials.The current development of GDY materials in various electrochemical fields especially in energy conversion,energy storage,and catalysis is mainly summarized.Moreover,the potential development prospects are also discussed. 相似文献
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Xiangyu Meng Chao Ma Luozhen Jiang Rui Si Xianguang Meng Yunchuan Tu Liang Yu Xinhe Bao Dehui Deng 《Angewandte Chemie (International ed. in English)》2020,59(26):10502-10507
Perturbing the electronic structure of the MoS2 basal plane by confining heteroatoms offers the opportunity to trigger in‐plane activity for the hydrogen evolution reaction (HER). The key challenge consists of inducing the optimum HER activity by controlling the type and distribution of confined atoms. A distance synergy of MoS2‐confined single‐atom rhodium is presented, leading to an ultra‐high HER activity at the in‐plane S sites adjacent to the rhodium. By optimizing the distance between the confined Rh atoms, an ultra‐low overpotential of 67 mV is achieved at a current density of 10 mA cm?2 in acidic solution. Experiments and first‐principles calculations demonstrate a unique distance synergy between the confined rhodium atoms in tuning the reactivity of neighboring in‐plane S atoms, which presents a volcanic trend with the inter‐rhodium distance. This study provides a new strategy to tailor the activity of MoS2 surface via modulating the distance between confined single atoms. 相似文献
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Zhijun Chen Dr. Yutao Cui Chunhui Ye Dr. Liyao Liu Xiaoyu Wu Dr. Yimeng Sun Prof. Wei Xu Prof. Daoben Zhu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(56):12868-12873
Metal-bis(dithiolene) is one of the most promising structures showing redox activity, excellent electron transport and magnetic properties as well as catalytic activities. Perthiolated coronene (PTC), an emerging highly symmetric ligand containing the smallest graphene nanoplate was employed to manufacture a hybrid material with fused metal-bis(dithiolene) and graphene nanoplate, and it has been demonstrated as an efficient strategy for the construction of multifunctional materials recently. Herein, Co-PTC, a 2D MOF containing Co-bis(dithiolene) and coronene units is prepared via a homogeneous reaction for the first time as powder samples, which are bar-shaped microparticles composed of nanosheets. A neutral formula of [Co3(C24S12)]n is verified for Co-PTC. Co-PTC plays an ultrahigh conductivity of approximately 45 S cm−1 at room temperature as compressed samples, which is among the highest value ever reported for the compressed powder samples of conducting MOFs. Moreover, Co-PTC exhibits good electrocatalytic performance in the hydrogen evolution reaction (HER) with a Tafel slope of 189 mV decade−1 and an operating overpotential of 227 mV at 10 mA cm−1 with pH=0, as well as a remarkable stability in the extremely acidic aqueous solutions, which is the best hydrogen evolution properties among metal–organic compounds. 相似文献
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Hierarchical β‐Mo2C Nanotubes Organized by Ultrathin Nanosheets as a Highly Efficient Electrocatalyst for Hydrogen Production 下载免费PDF全文
Fei‐Xiang Ma Dr. Hao Bin Wu Dr. Bao Yu Xia Prof. Cheng‐Yan Xu Prof. Xiong Wen Lou 《Angewandte Chemie (International ed. in English)》2015,54(51):15395-15399
Production of hydrogen by electrochemical water splitting has been hindered by the high cost of precious metal catalysts, such as Pt, for the hydrogen evolution reaction (HER). In this work, novel hierarchical β‐Mo2C nanotubes constructed from porous nanosheets have been fabricated and investigated as a high‐performance and low‐cost electrocatalyst for HER. An unusual template‐engaged strategy has been utilized to controllably synthesize Mo‐polydopamine nanotubes, which are further converted into hierarchical β‐Mo2C nanotubes by direct carburization at high temperature. Benefitting from several structural advantages including ultrafine primary nanocrystallites, large exposed surface, fast charge transfer, and unique tubular structure, the as‐prepared hierarchical β‐Mo2C nanotubes exhibit excellent electrocatalytic performance for HER with small overpotential in both acidic and basic conditions, as well as remarkable stability. 相似文献