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1.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(44):13882-13886
Single‐atom catalysts (SACs) have exhibited high activities for the hydrogen evolution reaction (HER) electrocatalysis in acidic or alkaline media, when they are used with binders on cathodes. However, to date, no SACs have been reported for the HER electrocatalysis in neutral media. We demonstrate a potential‐cycling method to synthesize a catalyst comprising single Pt atoms on CoP‐based nanotube arrays supported by a Ni foam, termed PtSA‐NT‐NF. This binder‐free catalyst is centimeter‐scale and scalable. It is directly used as HER cathodes, whose performances at low and high current densities in phosphate buffer solutions (pH 7.2) are comparable to and better than, respectively, those of commercial Pt/C. The Pt mass activity of PtSA‐NT‐NF is 4 times of that of Pt/C, and its electrocatalytic stability is also better than that of Pt/C. This work provides a large‐scale production strategy for binder‐free Pt SAC electrodes for efficient HER in neutral media. 相似文献
2.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(49):15800-15804
Realization of the hydrogen economy relies on effective hydrogen production, storage, and utilization. The slow kinetics of hydrogen evolution and oxidation reaction (HER/HOR) in alkaline media limits many practical applications involving hydrogen generation and utilization, and how to overcome this fundamental limitation remains debatable. Here we present a kinetic study of the HOR on representative catalytic systems in alkaline media. Electrochemical measurements show that the HOR rate of Pt‐Ru/C and Ru/C systems is decoupled to their hydrogen binding energy (HBE), challenging the current prevailing HBE mechanism. The alternative bifunctional mechanism is verified by combined electrochemical and in situ spectroscopic data, which provide convincing evidence for the presence of hydroxy groups on surface Ru sites in the HOR potential region and its key role in promoting the rate‐determining Volmer step. The conclusion presents important references for design and selection of HOR catalysts. 相似文献
3.
Advancing the Electrochemistry of the Hydrogen‐Evolution Reaction through Combining Experiment and Theory
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Dr. Yao Zheng Dr. Yan Jiao Prof. Mietek Jaroniec Prof. Shi Zhang Qiao 《Angewandte Chemie (International ed. in English)》2015,54(1):52-65
The electrocatalytic hydrogen‐evolution reaction (HER), as the main step of water splitting and the cornerstone of exploring the mechanism of other multi‐electron transfer electrochemical processes, is the subject of extensive studies. A large number of high‐performance electrocatalysts have been developed for HER accompanied by recent significant advances in exploring its electrochemical nature. Herein we present a critical appraisal of both theoretical and experimental studies of HER electrocatalysts with special emphasis on the electronic structure, surface (electro)chemistry, and molecular design. It addresses the importance of correlating theoretical calculations and electrochemical measurements toward better understanding of HER electrocatalysis at the atomic level. Fundamental concepts in the computational quantum chemistry and its relation to experimental electrochemistry are also presented along with some featured examples. 相似文献
4.
Dr. Chuangang Hu Prof. Liming Dai 《Angewandte Chemie (International ed. in English)》2016,55(39):11736-11758
Besides their use in fuel cells for energy conversion through the oxygen reduction reaction (ORR), carbon‐based metal‐free catalysts have also been demonstrated to be promising alternatives to noble‐metal/metal oxide catalysts for the oxygen evolution reaction (OER) in metal–air batteries for energy storage and for the splitting of water to produce hydrogen fuels through the hydrogen evolution reaction (HER). This Review focuses on recent progress in the development of carbon‐based metal‐free catalysts for the OER and HER, along with challenges and perspectives in the emerging field of metal‐free electrocatalysis. 相似文献
5.
Xiaojun Guo Ni Wang Xialiang Li Zongyao Zhang Jianping Zhao Wanjie Ren Shuping Ding Gelun Xu Jianfeng Li Ulf‐Peter Apfel Wei Zhang Rui Cao 《Angewandte Chemie (International ed. in English)》2020,59(23):8941-8946
Several H?H bond forming pathways have been proposed for the hydrogen evolution reaction (HER). Revealing these HER mechanisms is of fundamental importance for the rational design of catalysts and is also extremely challenging. Now, an unparalleled example of switching between homolytic and heterolytic HER mechanisms is reported. Three nickel(II) porphyrins were designed and synthesized with distinct steric effects by introducing bulky amido moieties to ortho‐ or para‐positions of the meso‐phenyl groups. These porphyrins exhibited different catalytic HER behaviors. For these Ni porphyrins, although their 1e‐reduced forms are active to reduce trifluoroacetic acid, the resulting Ni hydrides (depending on the steric effects of porphyrin rings) have different pathways to make H2. Understanding HER processes, especially controllable switching between homolytic and heterolytic H?H bond formation pathways through molecular engineering, is unprecedented in electrocatalysis. 相似文献
6.
Guoqiang Zhao Xingyong Wang Shaolan Wang Kun Rui Yaping Chen Haibo Yu Jing Ma Shi Xue Dou Wenping Sun 《化学:亚洲杂志》2019,14(2):301-306
Electrochemical water splitting for hydrogen generation is a vital part for the prospect of future energy systems, however, the practical utilization relies on the development of highly active and earth‐abundant catalysts to boost the energy conversion efficiency as well as reduce the cost. Molybdenum diselenide (MoSe2) is a promising nonprecious metal‐based electrocatalyst for hydrogen evolution reaction (HER) in acidic media, but it exhibits inferior alkaline HER kinetics in great part due to the sluggish water adsorption/dissociation process. Herein, the alkaline HER kinetics of MoSe2 is substantially accelerated by heteroatom doping with transition metal ions. Specifically, the Ni‐doped MoSe2 nanosheets exhibit the most impressive catalytic activity in terms of lower overpotential and larger exchange current density. The density functional theory (DFT) calculation results reveal that Ni/Co doping plays a key role in facilitating water adsorption as well as optimizing hydrogen adsorption. The present work paves a new way to the development of low‐cost and efficient electrocatalysts towards alkaline HER. 相似文献
7.
Yuanmeng Zhao Xuewei Wang Zhen Li Pingping Zhao Congliang Tao Gongzhen Cheng Wei Luo 《中国化学快报》2022,33(2):1065-1069
Exploring highly efficient electrocatalysts and understanding the reaction mechanisms for hydrogen electrocatalysis,including hydrogen oxidation reaction (HOR) and hydrogen evolution reaction (HER) in alkaline media are conducive to the conversion of hydrogen energy.Herein,we reported a new strategy to boost the HER/HOR performances of ruthenium (Ru) nanoparticles through nitrogen (N) modification.The obtained N-Ru/C exhibit remarkable catalytic performance,with normalized HOR exchange current d... 相似文献
8.
Dimeric [Mo2S12]2− Cluster: A Molecular Analogue of MoS2 Edges for Superior Hydrogen‐Evolution Electrocatalysis
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Zhongjie Huang Wenjia Luo Lu Ma Mingzhe Yu Xiaodi Ren Mingfu He Shane Polen Kevin Click Benjamin Garrett Prof. Jun Lu Prof. Khalil Amine Prof. Christopher Hadad Prof. Weilin Chen Prof. Aravind Asthagiri Prof. Yiying Wu 《Angewandte Chemie (International ed. in English)》2015,54(50):15181-15185
Proton reduction is one of the most fundamental and important reactions in nature. MoS2 edges have been identified as the active sites for hydrogen evolution reaction (HER) electrocatalysis. Designing molecular mimics of MoS2 edge sites is an attractive strategy to understand the underlying catalytic mechanism of different edge sites and improve their activities. Herein we report a dimeric molecular analogue [Mo2S12]2?, as the smallest unit possessing both the terminal and bridging disulfide ligands. Our electrochemical tests show that [Mo2S12]2? is a superior heterogeneous HER catalyst under acidic conditions. Computations suggest that the bridging disulfide ligand of [Mo2S12]2? exhibits a hydrogen adsorption free energy near zero (?0.05 eV). This work helps shed light on the rational design of HER catalysts and biomimetics of hydrogen‐evolving enzymes. 相似文献
9.
Jiao Zhao Dr. Menglin Wang Yu Peng Jie Ni Sunpei Hu Prof. Dr. Jie Zeng Prof. Dr. Qianjin Chen 《Angewandte Chemie (International ed. in English)》2023,62(30):e202304424
Tuning the surface strain of heterogeneous catalysts is recognized as a powerful strategy for tailoring their catalytic activity. However, a clear understanding of the strain effect in electrocatalysis at single-particle resolution is still lacking. Here, we explore the electrochemical hydrogen evolution reaction (HER) of single Pd octahedra and icosahedra with the same surface bounded {111} crystal facet and similar sizes using scanning electrochemical cell microscopy (SECCM). It is revealed that tensilely strained Pd icosahedra display significantly superior HER electrocatalytic activity. The estimated turnover frequency at −0.87 V vs RHE on Pd icosahedra is about two times higher than that on Pd octahedra. Our single-particle electrochemistry study using SECCM at Pd nanocrystals unambiguously highlights the importance of tensile strain on electrocatalytic activity and may offer new strategy for understanding the fundamental relationship between surface strain and reactivity. 相似文献
10.
Xinqun Zhang Jian Gao Yukun Xiao Jiaqi Wang Guoqiang Sun Yang Zhao Liangti Qu 《化学:亚洲杂志》2020,15(15):2271-2281
Benefiting from unique excellent physical and chemical characteristics, graphene has attracted widespread attention in the application of electrocatalysis. As a promising candidate, graphene is usually regulated with surface defects, heteroatoms, metal atoms and other active materials through covalent or non‐covalent bonds to substitute for noble metal catalysts, which has not been targeted in a report yet. In this review, we summarize the recent advances of approaches for engineering graphene‐based electrocatalysts and emphasize the corresponding electrocatalytic active sites in various electrocatalysis circumstances, such as electrocatalytic hydrogen evolution reaction (HER), oxygen evolution reaction (OER), oxygen reduction reaction (ORR), etc. The opportunities and challenges in the future development of graphene‐based catalysts are also discussed. 相似文献
11.
Sammy Onajah Dr. Rajib Sarkar Md. Shafiul Islam Marja Lalley Dr. Kishwar Khan Dr. Muslum Demir Dr. Hani Nasser Abdelhamid Dr. Ahmed A. Farghaly 《Chemical record (New York, N.Y.)》2024,24(4):e202300234
Silica-derived nanostructured catalysts (SDNCs) are a class of materials synthesized using nanocasting and templating techniques, which involve the sacrificial removal of a silica template to generate highly porous nanostructured materials. The surface of these nanostructures is functionalized with a variety of electrocatalytically active metal and non-metal atoms. SDNCs have attracted considerable attention due to their unique physicochemical properties, tunable electronic configuration, and microstructure. These properties make them highly efficient catalysts and promising electrode materials for next generation electrocatalysis, energy conversion, and energy storage technologies. The continued development of SDNCs is likely to lead to new and improved electrocatalysts and electrode materials. This review article provides a comprehensive overview of the recent advances in the development of SDNCs for electrocatalysis and energy storage applications. It analyzes 337,061 research articles published in the Web of Science (WoS) database up to December 2022 using the keywords “silica”, “electrocatalysts”, “ORR”, “OER”, “HER”, “HOR”, “CO2RR”, “batteries”, and “supercapacitors”. The review discusses the application of SDNCs for oxygen reduction reaction (ORR), oxygen evolution reaction (OER), hydrogen evolution reaction (HER), carbon dioxide reduction reaction (CO2RR), supercapacitors, lithium-ion batteries, and thermal energy storage applications. It concludes by discussing the advantages and limitations of SDNCs for energy applications. 相似文献
12.
Jin‐Xian Feng Han Xu Yu‐Tao Dong Xue‐Feng Lu Ye‐Xiang Tong Prof. Gao‐Ren Li 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(11):3006-3010
TiO2 Co nanotubes decorated with nanodots (TiO2 NDs/Co NSNTs‐CFs) are reported as high‐performance earth‐abundant electrocatalysts for the hydrogen evolution reaction (HER) in alkaline solution. TiO2 NDs/Co NSNTs can promote water adsorption and optimize the free energy of hydrogen adsorption. More importantly, the absorbed water can be easily activated in the presence of the TiO2–Co hybrid structure. These advantages will significantly promote HER. TiO2 NDs/Co NSNTs‐CFs as electrocatalysts show a high catalytic performance towards HER in alkaline solution. This study will open up a new avenue for designing and fabricating low‐cost high‐performance HER catalysts. 相似文献
13.
14.
Phase and Interface Engineering of Platinum–Nickel Nanowires for Efficient Electrochemical Hydrogen Evolution
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Pengtang Wang Kezhu Jiang Prof. Gongming Wang Prof. Jianlin Yao Prof. Xiaoqing Huang 《Angewandte Chemie (International ed. in English)》2016,55(41):12859-12863
The design of high‐performance electrocatalysts for the alkaline hydrogen evolution reaction (HER) is highly desirable for the development of alkaline water electrolysis. Phase‐ and interface‐engineered platinum–nickel nanowires (Pt‐Ni NWs) are highly efficient electrocatalysts for alkaline HER. The phase and interface engineering is achieved by simply annealing the pristine Pt‐Ni NWs under a controlled atmosphere. Impressively, the newly generated nanomaterials exhibit superior activity for the alkaline HER, outperforming the pristine Pt‐Ni NWs and commercial Pt/C, and also represent the best alkaline HER catalysts to date. The enhanced HER activities are attributed to the superior phase and interface structures in the engineered Pt‐Ni NWs. 相似文献
15.
Yueyu Tong Haipeng Guo Daolan Liu Xiao Yan Panpan Su Ji Liang Si Zhou Jian Liu Gao Qing Lu Shi Xue Dou 《Angewandte Chemie (International ed. in English)》2020,59(19):7356-7361
The electrochemical nitrogen reduction reaction (NRR) is a promising energy‐efficient and low‐emission alternative to the traditional Haber–Bosch process. Usually, the competing hydrogen evolution reaction (HER) and the reaction barrier of ambient electrochemical NRR are significant challenges, making a simultaneous high NH3 formation rate and high Faradic efficiency (FE) difficult. To give effective NRR electrocatalysis and suppressed HER, the surface atomic structure of W18O49, which has exposed active W sites and weak binding for H2, is doped with Fe. A high NH3 formation rate of 24.7 μg h?1 mgcat?1 and a high FE of 20.0 % are achieved at an overpotential of only ?0.15 V versus the reversible hydrogen electrode. Ab initio calculations reveal an intercalation‐type doping of Fe atoms in the tunnels of the W18O49 crystal structure, which increases the oxygen vacancies and exposes more W active sites, optimizes the nitrogen adsorption energy, and facilitates the electrocatalytic NRR. 相似文献
16.
Hui Chen Xuan Ai Wang Liu Zhoubing Xie Weiqiang Feng Wei Chen Xiaoxin Zou 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(33):11531-11535
The fundamental understanding and rational manipulation of catalytic site preference at extended solid surfaces is crucial in the search for advanced catalysts. Herein we find that the Ru top sites at metallic ruthenium surface have efficient Pt‐like activity for the hydrogen evolution reaction (HER), but they are subordinate to their adjacent, less active Ru3‐hollow sites due to the stronger hydrogen‐binding ability of the latter. We also present an interstitial incorporation strategy for the promotion of the Ru top sites from subordinate to dominant character, while maintaining Pt‐like catalytic activity. Our combined theoretical and experimental studies further identify intermetallic RuSi as a highly active, non‐Pt material for catalyzing the HER, because of its suitable electronic structure governed by a good balance of ligand and strain effects. 相似文献
17.
氢气因为其高质量比活性,环境友好等特点,被公认为是一种很有希望替代化石能源的可再生能源.其中,碱性条件电解水被认为是可大规模生产氢气的技术之一.但氢气析出反应在碱性条件反应速率缓慢,为提升氢气析出反应速率,因此研究者们设计和制备了大量的材料.本文归纳了有效促进碱性条件氢气析出反应速率的关键材料——层状过渡金属氢氧化物的重要研究进展.首先,基于过渡金属氢氧化物的结构,阐述了过渡金属氢氧化物与氢气析出反应活性材料间的协同催化机理.接着,以提升协同催化作用为中心,归纳了基于过渡金属氢氧化物的氢气析出反应催化剂和电极的最近研究进展,分别包含过渡金属氢氧化物和氢气析出反应活性材料的种类、结构、形貌及其相互作用.此外,本文从高活性和长寿命的催化剂和电极设计出发,归纳了最近基于过渡金属氢氧化物的催化剂和电极在水分解领域的进展.最后,本文总结和展望了电解水制氢技术的未来应用和发展中不可避免的一些问题与挑战.目前,应用于氢析出反应的过渡金属氢氧化物主要集中于镍基、钴基和铁基氢氧化物和其双金属氢氧化物,为层状水滑石结构.因为上述过渡金属氢氧化物弱的氢吸附,所以其析氢活性非常低.但是过渡金属氢氧化物对氢氧根... 相似文献
18.
Hui Chen Xuan Ai Wang Liu Zhoubing Xie Weiqiang Feng Wei Chen Xiaoxin Zou 《Angewandte Chemie (International ed. in English)》2019,58(33):11409-11413
The fundamental understanding and rational manipulation of catalytic site preference at extended solid surfaces is crucial in the search for advanced catalysts. Herein we find that the Ru top sites at metallic ruthenium surface have efficient Pt‐like activity for the hydrogen evolution reaction (HER), but they are subordinate to their adjacent, less active Ru3‐hollow sites due to the stronger hydrogen‐binding ability of the latter. We also present an interstitial incorporation strategy for the promotion of the Ru top sites from subordinate to dominant character, while maintaining Pt‐like catalytic activity. Our combined theoretical and experimental studies further identify intermetallic RuSi as a highly active, non‐Pt material for catalyzing the HER, because of its suitable electronic structure governed by a good balance of ligand and strain effects. 相似文献
19.
Ting Ouyang Ya‐Qian Ye Chun‐Yan Wu Kang Xiao Zhao‐Qing Liu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(15):4977-4982
Herein, we demonstrate the use of heterostructures comprised of Co/β‐Mo2C@N‐CNT hybrids for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in an alkaline electrolyte. The Co can not only create a well‐defined heterointerface with β‐Mo2C but also overcomes the poor OER activity of β‐Mo2C, thus leading to enhanced electrocatalytic activity for HER and OER. DFT calculations further proved that cooperation between the N‐CNTs, Co, and β‐Mo2C results in lower energy barriers of intermediates and thus greatly enhances the HER and OER performance. This study not only provides a simple strategy for the construction of heterostructures with nonprecious metals, but also provides in‐depth insight into the HER and OER mechanism in alkaline solution. 相似文献