共查询到20条相似文献,搜索用时 15 毫秒
1.
Zemin Sun Mengwei Yuan Kefan Shi Yuhui Liu Di Wang Dr. Caiyun Nan Dr. Huifeng Li Prof. Genban Sun Prof. Xiaojing Yang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(32):7244-7249
NiFe layered double hydroxides (LDHs) have been denoted as benchmark non-noble-metal electrocatalysts for the oxygen evolution reaction (OER). However, for laminates of NiFe LDHs, the edge sites are active, but the basal plane is inert, leading to underutilization as catalysts for the OER. Herein, for the first time, light and electron-deficient Li ions are intercalated into the basal plane of NiFe LDHs. The results of theoretical calculations and experiments both showed that electrons would be transferred from near Ni2+ to the surroundings of Li+, resulting in electron-deficient properties of the Ni sites, which would function as “electron-hungry” sites, to enhance surface adsorption of electron-rich oxygen-containing groups, which would enhance the effective activity for the OER. As demonstrated by the catalytic performance, the Li−NiFe LDH electrodes showed an ultralow overpotential of only 298 mV at 50 mA cm−2, which was lower than that of 347 mV for initial NiFe LDHs and lower than that of 373 mV for RuO2. Reasonable intercalation adjustment effectively activates laminated Ni2+ sites and constructs the electron-deficient structure to enhance its electrocatalytic activity, which sheds light on the functional treatment of catalytic materials. 相似文献
2.
Wen-Jie Jiang Shuai Niu Tang Tang Qing-Hua Zhang Xiao-Zhi Liu Yun Zhang Yu-Yun Chen Prof. Ji-Hui Li Prof. Lin Gu Prof. Li-Jun Wan Prof. Jin-Song Hu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(23):6672-6677
The exploration of new efficient OER electrocatalysts based on nonprecious metals and the understanding of the relationship between activity and structure of electrocatalysts are important to advance electrochemical water oxidation. Herein, we developed an efficient OER electrocatalyst with nickel boride (Ni3B) nanoparticles as cores and nickel(II) borate (Ni-Bi) as shells (Ni-Bi@NB) via a very simple and facile aqueous reaction. This electrocatalyst exhibited a small overpotential of 302 mV at 10 mA cm−2 and Tafel slope of 52 mV dec−1. More interestingly, it was found that the OER activity of Ni-Bi@NB was closely dependent on the crystallinity of the Ni-Bi shells. The partially crystalline Ni-Bi catalyst exhibited much higher activity than the amorphous or crystalline analogues; this higher activity originated from the enhanced intrinsic activity of the catalytic sites. These findings open up opportunities to explore nickel(II) borates as a new class of efficient nonprecious metal OER electrocatalysts, and to improve the electrocatalyst performance by modulating their crystallinity. 相似文献
3.
《化学:亚洲杂志》2017,12(22):2956-2961
Developing efficient non‐noble metal and earth‐abundant electrocatalysts with tunable microstructures for overall water splitting is critical to promote clean energy technologies for a hydrogen economy. Herein, novel three‐dimensional (3D) flower‐like Ni2P composed of mesoporous nanoplates with controllable morphology and high surface area was prepared by a hydrothermal method and low‐temperature phosphidation as efficient electrocatalysts for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Compared with the urchin‐like Nix Py , the 3D flower‐like Ni2P with a diameter of 5 μm presented an efficient and stable catalytic performance in 0.5 m H2SO4, with a small Tafel slope of 79 mV dec−1 and an overpotential of about 240 mV at a current density of 10 mA cm−2 with a mass loading density of 0.283 mg cm−2. In addition, the catalyst also exhibited a remarkable performance for the OER in 1.0 m KOH electrolyte, with an overpotential of 320 mV to reach a current density of 10 mA cm−2 and a small Tafel slope of 72 mV dec−1. The excellent catalytic performance of the as‐prepared Ni2P may be ascribed to its novel 3D morphology with unique mesoporous structure. 相似文献
4.
Prof. Li An Dr. Hong Zhang Jiamin Zhu Prof. Shibo Xi Prof. Bolong Huang Mingzi Sun Prof. Yong Peng Prof. Pinxian Xi Prof. Chun-Hua Yan 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2023,135(3):e202214600
Designing active and stable oxygen evolution reaction (OER) catalysts are vitally important to various energy conversion devices. Herein, we introduce elements Ni and Mn into (Co)tet(Co2)octO4 nanosheets (NSs) at fixed geometrical sites, including Mnoct, Nioct, and Nitet, to optimize the initial geometrical structure and modulate the CoCo2O4 surface from oxygen-excess to oxygen-deficiency. The pristine (Ni,Mn)-(Co)tet(Co2)octO4 NSs shows excellent OER activity with an overpotential of 281.6 mV at a current density of 10 mA cm−2. Moreover, without damaging their initial activity, the activated (Act)-(Ni,Mn)-(Co)tet(Co2)octO4 NSs after surface reconstruction exhibit long-term stability of 100 h under 10 mA cm−2, 50 mA cm−2, or even 100 mA cm−2. The optimal balance between electroactivity and stability leads to remarkable OER performances, providing a pivotal guideline for designing ideal electrocatalysts and inspiring more works to focus on the dynamic change of each occupation site component. 相似文献
5.
《化学:亚洲杂志》2017,12(20):2694-2702
Iron–cobalt phosphomolybdate (FeCoPM12) nanoparticles, which are highly efficient catalytic materials for the oxygen evolution reaction (OER), were fabricated through a coprecipitation route. Compared with iron–cobalt hydroxide and state‐of‐the‐art RuO2 electrocatalysts, the as‐prepared FeCoPM12 sample exhibited robust OER catalytic activity with a low overpotential of 258 mV at a current density of 10 mA cm−2 and a small Tafel slope of 33 mV dec−1. Moreover, the as‐synthesized sample presented preferable stability and after 10 h at 1.52 V the current density degraded by merely 8.3 %. This is ascribed to the high electrochemical stability and small porous structure of FeCoPM12, which provide effective electron transmission and improve the catalytic performance for OER in alkaline media. 相似文献
6.
Xiaofang Bai Xiuping Zhang Yujiao Sun Mingcheng Huang Prof. Dr. Jiantao Fan Prof. Dr. Shaoyi Xu Prof. Dr. Hui Li 《Angewandte Chemie (International ed. in English)》2023,62(38):e202308704
To date, only a few noble metal oxides exhibit the required efficiency and stability as oxygen evolution reaction (OER) catalysts under the acidic, high-voltage conditions that exist during proton exchange membrane water electrolysis (PEMWE). The high cost and scarcity of these catalysts hinder the large-scale application of PEMWE. Here, we report a novel OER electrocatalyst for OER comprised of uniformly dispersed Ru clusters confined on boron carbon nitride (BCN) support. Compared to RuO2, our BCN-supported catalyst shows enhanced charge transfer. It displays a low overpotential of 164 mV at a current density of 10 mA cm−2, suggesting its excellent OER catalytic activity. This catalyst was able to operate continuously for over 12 h under acidic conditions, whereas RuO2 without any support fails in 1 h. Density functional theory (DFT) calculations confirm that the interaction between the N on BCN support and Ru clusters changes the adsorption capacity and reduces the OER energy barrier, which increases the electrocatalytic activity of Ru. 相似文献
7.
Cheng Wang Prof. Limin Qi 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(39):17372-17377
The development of transition-metal-oxides (TMOs)-based bifunctional catalysts toward efficient overall water splitting through delicate control of composition and structure is a challenging task. Herein, the rational design and controllable fabrication of unique heterostructured inter-doped ruthenium–cobalt oxide [(Ru–Co)Ox] hollow nanosheet arrays on carbon cloth is reported. Benefiting from the desirable compositional and structural advantages of more exposed active sites, optimized electronic structure, and interfacial synergy effect, the (Ru–Co)Ox nanoarrays exhibited outstanding performance as a bifunctional catalyst. Particularly, the catalyst showed a remarkable hydrogen evolution reaction (HER) activity with an overpotential of 44.1 mV at 10 mA cm−2 and a small Tafel slope of 23.5 mV dec−1, as well as an excellent oxygen evolution reaction (OER) activity with an overpotential of 171.2 mV at 10 mA cm−2. As a result, a very low cell voltage of 1.488 V was needed at 10 mA cm−2 for alkaline overall water splitting. 相似文献
8.
Xiaoliang Lu Jinzhi Zhou Jinxiu Zhao Prof. Dan Wu Xuejing Liu Prof. Xiang Ren Prof. Qin Wei Prof. Huangxian Ju 《Chemphyschem》2023,24(20):e202300536
The electrocatalytic nitrate reduction reaction (NO3−RR) enables the reduction of nitrate to ammonium ions under ambient conditions. It was considered as an alternative reaction for the production of ammonia (NH3) in recent years. In this paper, we report that the Fe doping CoS2 nanoarrays can effectively catalyze the formation of NH3 from nitrate (NO3−) under ambient conditions. This is mainly due to the increase of the NO3− reaction active site by Fe doping and the porous nanostructure of the catalyst, which greatly improves the catalytic activity. Specifically, at −0.9 V vs. RHE, the NH3 yield rate (RNH3) of Fe−CoS2/CC is 17.8×10−2 mmol h−1 cm−2 with Faraday Efficiency (FE) of 88.93 %. Besides, such catalyst shows good durability and catalytic stability, which provides the possibility for the future application of electrocatalytic NH3 production. 相似文献
9.
Xiuxiu Zhang Chenyu Yang Chen Gong Meihuan Liu Wanlin Zhou Hui Su Feifan Yu Fengchun Hu Qinghua Liu Shiqiang Wei 《Angewandte Chemie (International ed. in English)》2023,62(33):e202308082
Synthesis of highly active and durable oxygen evolution reaction (OER) catalysts applied in acidic water electrolysis remains a grand challenge. Here, we construct a type of high-loading iridium single atom catalysts with tunable d-band holes character (h-HL−Ir SACs, ∼17.2 wt % Ir) realized in the early OER operation stages. The in situ X-ray absorption spectroscopy reveals that the quantity of the d-band holes of Ir active sites can be fast increased by 0.56 unit from the open circuit to a low working potential of 1.35 V. More remarkably, in situ synchrotron infrared and Raman spectroscopies demonstrate the quick accumulation of *OOH and *OH intermediates over holes-modulated Ir sites in the early reaction voltages, achieving a rapid OER kinetics. As a result, this well-designed h-HL−Ir SACs exhibits superior performance for acidic OER with overpotentials of 216 mV @10 mA cm−2 and 259 mV @100 mA cm−2, corresponding to a small Tafel slope of 43 mV dec−1. The activity of catalyst shows no evident attenuation after 60 h operation in acidic environment. This work provides some useful hints for the design of superior acidic OER catalysts. 相似文献
10.
Jing Gao Liu Yang Di Wang Prof. Dr. Dapeng Cao 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(18):4112-4119
Hydrogen energy is considered as one of the ideal clean energies for solving the energy shortage and environmental issues, and developing highly efficient electrocatalysts for overall water splitting to produce hydrogen is still a huge challenge. Herein, for the first time, Ru-doped Cu2+1O vertically arranged nanotube arrays in situ grown on Cu foam (Ru/Cu2+1O NT/CuF) are reported and further investigated for their catalytic properties for overall water splitting. The Ru/Cu2+1O NT/CuF presents ultrahigh catalytic activities for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in alkaline conditions, and it exhibits a small overpotential of 32 mV at 10 mA cm−2 in the HER, and only needs 210 mV overpotential to achieve a current density of 10 mA cm−2 in the OER. Importantly, the alkaline electrolyzer using Ru/Cu2+1O NT/CuF as a bifunctional electrocatalyst only needs 1.53 V voltage to deliver a current density of 10 mA cm−2, which is much lower than the benchmark of IrO2(+)/Pt(−) counterpart (1.64 V at 10 mA cm−2). The excellent performance of the Ru/Cu2+1O NT/CuF catalyst is attributed to its high conductive substrate and special Ru-doped nanotube structure, which provides a high electrochemical active surface area and 3D gas diffusion channel. 相似文献
11.
Dong He Xianyin Song Wenqing Li Chongyang Tang Jiangchao Liu Zunjian Ke Prof. Changzhong Jiang Prof. Xiangheng Xiao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(17):6996-7002
Despite the fact that many strategies have been developed to improve the efficiency of the oxygen evolution reaction (OER), the precise modulation of the surface electronic properties of catalysts to improve their catalytic activity is still challenging. Herein, we demonstrate that the surface active electron density of Co3O4 can be effectively regulated by an argon-ion irradiation method. X-ray photoelectron and synchrotron x-ray absorption spectroscopy, UV photoelectron spectrometry, and DFT calculations show that the surface active electron density band center of Co3O4 has been upshifted, leading to a significantly enhanced absorption capability of the oxo group. The optimized Co3O4-based catalysts exhibit an excellent overpotential of 260 mV at 10 mA cm−2 and Tafel slope of 54 mV dec−1, superior to the capability of the benchmark RuO2, representing one of the best Co-based OER catalysts. This approach could guide the future rational design and discovery of ideal electrocatalysts. 相似文献
12.
Strong‐Coupled Cobalt Borate Nanosheets/Graphene Hybrid as Electrocatalyst for Water Oxidation Under Both Alkaline and Neutral Conditions 下载免费PDF全文
Pengzuo Chen Kun Xu Tianpei Zhou Yun Tong Junchi Wu Han Cheng Xiuli Lu Hui Ding Prof. Changzheng Wu Prof. Yi Xie 《Angewandte Chemie (International ed. in English)》2016,55(7):2488-2492
Developing highly active catalysts for the oxygen evolution reaction (OER) is of paramount importance for designing various renewable energy storage and conversion devices. Herein, we report the synthesis of a category of Co‐Pi analogue, namely cobalt‐based borate (Co‐Bi) ultrathin nanosheets/graphene hybrid by a room‐temperature synthesis approach. Benefiting from the high surface active sites exposure yield, enhanced electron transfer capacity, and strong synergetic coupled effect, this Co‐Bi NS/G hybrid shows high catalytic activity with current density of 10 mA cm?2 at overpotential of 290 mV and Tafel slope of 53 mV dec?1 in alkaline medium. Moreover, Co‐Bi NS/G electrocatalysts also exhibit promising performance under neutral conditions, with a low onset potential of 235 mV and high current density of 14.4 mA cm?2 at 1.8 V, which is the best OER performance among well‐developed Co‐based OER electrocatalysts to date. Our finding paves a way to develop highly active OER electrocatalysts. 相似文献
13.
Chi Zhang Dr. Chen Zhang Yunchao Xie Jheng-Wun Su Dr. Xiaoqing He John D. Demaree Mark H. Griep Prof. Jerry L. Atwood Prof. Jian Lin 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(16):4036-4039
An iron oxide decorated nickel iron alloy nanoparticle/porous graphene hybrid exhibits high electrocatalytic activity and excellent durability toward oxygen evolution reaction (OER). It displays a low overpotential of 274 mV at 10 mA cm−2, and low Tafel slope of 37 mV dec−1, showing a superior performance to the state-of-the-art RuO2 OER electrocatalyst. 相似文献
14.
Da-Huan Li Xiao-Yue Zhang Jiang-Quan Lv Ping-Wei Cai Yan-Qiong Sun Prof. Dr. Cai Sun Prof. Dr. Shou-Tian Zheng 《Angewandte Chemie (International ed. in English)》2023,62(46):e202312706
Inspired by the metal-oxo cluster structural feature and charge separation behaviour of the oxygen evolving center (OEC) in photosystem II (PS-II) under photoirradiation, a new crystalline photochromic polyoxomolybdate, MV2[β-Mo8O26] ( 1 , MV=methyl viologen cation), is designed as a biomimetic oxygen evolution reaction (OER) catalyst in neutral electrolytes. After photoinduced electron transfer (PIET) with colour change from colourless to grey, it remains in an ultra-stable charge-separated state over a year under ambient conditions. The observed overpotential at 10 mA ⋅ cm−2 and Tafel slope decrease by 49 mV and 62.8 mV ⋅ dec−1 after coloration, respectively. The outstanding OER performance of the coloured state in neutral electrolytes even outperforms the commercial RuO2 benchmark. Experimental and theoretical studies show that oxygen holes within polyanions after irradiation serve as sites for enhancing direct O−O coupling, thus effectively promoting OER. This is the first successful application of electron-transfer photochromism to realize OER activity gain. 相似文献
15.
A Molecular Approach to Manganese Nitride Acting as a High Performance Electrocatalyst in the Oxygen Evolution Reaction 下载免费PDF全文
Carsten Walter Dr. Prashanth W. Menezes Steven Orthmann Jona Schuch Paula Connor Dr. Bernhard Kaiser Prof. Dr. Martin Lerch Prof. Dr. Matthias Driess 《Angewandte Chemie (International ed. in English)》2018,57(3):698-702
The scalable synthesis of phase‐pure crystalline manganese nitride (Mn3N2) from a molecular precursor is reported. It acts as a superiorly active and durable electrocatalyst in the oxygen evolution reaction (OER) from water under alkaline conditions. While electrophoretically deposited Mn3N2 on fluorine tin oxide (FTO) requires an overpotential of 390 mV, the latter is substantially decreased to merely 270 mV on nickel foam (NF) at a current density of 10 mA cm?2 with a durability of weeks. The high performance of this material is due to the rapid transformation of manganese sites at the surface of Mn3N2 into an amorphous active MnOx overlayer under operation conditions intimately connected with metallic Mn3N2, which increases the charge transfer from the active catalyst surface to the electrode substrates and thus outperforms the electrocatalytic activity in comparison to solely MnOx‐based OER catalysts. 相似文献
16.
采用一步水热法,通过引入载体碳球(CSs)和表面活性剂CTAB,将二硫化钴(CoS_2)纳米颗粒均匀负载在CSs表面.相比于单独的CoS_2,改性后CSs担载的CoS_2(CoS_2/A-CSs)展现出了更好的电催化活性.在电解液为0.5mol/L H_2SO_4溶液中,电流密度为10 mA·cm~(-2)条件下,其析氢反应过电位仅为154 mV.经过12 h的稳定性测试,CoS_2/A-CSs析氢反应过电位为180 mV,这表明其仍具有良好的电化学催化析氢反应活性.这种复合电催化剂的优良性能主要归因于CSs的高导电性和其对CoS_2纳米颗粒的均匀分散;此外,CTAB的引入,促使CSs与CoS_2之间结合的更加紧密,进而加快了活性位点间的电子传导. 相似文献
17.
Yuyin Wang Yan Wang Li Zhang Prof. Dr. Chun‐Sen Liu Prof. Dr. Huan Pang 《化学:亚洲杂志》2019,14(16):2790-2795
To realize the effective conversion of renewable energy through water decomposition, efficient electrocatalysts for the oxygen evolution reaction (OER) are essential. In this article, PBA@POM was successfully prepared with a Prussian blue analogue (PBA) as the initial structure. A facile hydrothermal process is reported for obtaining PBA@POM by etching the cubic PBA with a strong Brønsted acid, H3PMo12O40 (HPMo). The hollow cube structure not only exposes more active sites but also promotes electron transport, which results in excellent electrocatalytic activity for the OER. Compared with the PBA, which initially simply adhered to POM, the optimum PBA@POM hybrids display remarkably enhanced OER catalytic activity, with an almost constant overpotential of 440 mV at a current density of 10 mA cm?2 and a small Tafel slope (23.45 mV dec?1). The facilely prepared PBA@POM with good electrochemical activity and stability promises great potential for the OER. 相似文献
18.
Pengzuo Chen Kun Xu Zhiwei Fang Yun Tong Junchi Wu Xiuli Lu Xu Peng Hui Ding Changzheng Wu Yi Xie 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2015,127(49):14923-14927
Designing highly efficient electrocatalysts for oxygen evolution reaction (OER) plays a key role in the development of various renewable energy storage and conversion devices. In this work, we developed metallic Co4N porous nanowire arrays directly grown on flexible substrates as highly active OER electrocatalysts for the first time. Benefiting from the collaborative advantages of metallic character, 1D porous nanowire arrays, and unique 3D electrode configuration, surface oxidation activated Co4N porous nanowire arrays/carbon cloth achieved an extremely small overpotential of 257 mV at a current density of 10 mA cm−2, and a low Tafel slope of 44 mV dec−1 in an alkaline medium, which is the best OER performance among reported Co‐based electrocatalysts to date. Moreover, in‐depth mechanistic investigations demonstrate the active phases are the metallic Co4N core inside with a thin cobalt oxides/hydroxides shell during the OER process. Our finding introduces a new concept to explore the design of high‐efficiency OER electrocatalysts. 相似文献
19.
Dr. Yang Li Tingting Bo Dr. Shouwei Zuo Dr. Guikai Zhang Dr. Xiaojuan Zhao Prof. Wei Zhou Dr. Xin Wu Guoxiang Zhao Dr. Huawei Huang Prof. Lirong Zheng Prof. Jing Zhang Prof. Huabin Zhang Prof. Jian Zhang 《Angewandte Chemie (International ed. in English)》2023,62(41):e202309341
Developing efficient electrocatalysts for the oxygen evolution reaction (OER) is paramount to the energy conversion and storage devices. However, the structural complexity of heterogeneous electrocatalysts makes it a great challenge to elucidate the dynamic structural evolution and OER mechanisms. Here, we develop a controllable atom-trapping strategy to extract isolated Mo atom from the amorphous MoOx-decorated CoSe2 (a-MoOx@CoSe2) pre-catalyst into Co-based oxyhydroxide (Mo-CoOOH) through an ultra-fast self-reconstruction process during the OER process. This conceptual advance has been validated by operando characterizations, which reveals that the initially rapid Mo leaching can expedite the dynamic reconstruction of pre-catalyst, and simultaneously trap Mo species in high oxidation state into the lattice of in situ generated CoOOH support. Impressively, the OER kinetics of CoOOH has been greatly accelerated after the reverse decoration of Mo species, in which the Mo-CoOOH affords a markedly decreased overpotential of 297 mV at the current density of 100 mA cm−2. Density functional theory (DFT) calculations demonstrate that the Co species have been greatly activated via the effective electron coupling with Mo species in high oxidation state. These findings open new avenues toward directly synthesizing atomically dispersed electrocatalysts for high-efficiency water splitting. 相似文献
20.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(35):10642-10646
A highly active FeSe2 electrocatalyst for durable overall water splitting was prepared from a molecular 2Fe‐2Se precursor. The as‐synthesized FeSe2 was electrophoretically deposited on nickel foam and applied to the oxygen and hydrogen evolution reactions (OER and HER, respectively) in alkaline media. When used as an oxygen‐evolution electrode, a low 245 mV overpotential was achieved at a current density of 10 mA cm−2, representing outstanding catalytic activity and stability because of Fe(OH)2/FeOOH active sites formed at the surface of FeSe2. Remarkably, the system is also favorable for the HER. Moreover, an overall water‐splitting setup was fabricated using a two‐electrode cell, which displayed a low cell voltage and high stability. In summary, the first iron selenide material is reported that can be used as a bifunctional electrocatalyst for the OER and HER, as well as overall water splitting. 相似文献