共查询到20条相似文献,搜索用时 31 毫秒
1.
Jian Bao Wenjun Liu Junfeng Xie Li Xu Meili Guan Fengcai Lei Yan Zhao Yunpeng Huang Jiexiang Xia Huaming Li 《化学:亚洲杂志》2019,14(3):480-485
Developing highly active, stable and robust electrocatalysts based on earth‐abundant elements for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is important for many renewable energy conversion processes. Herein, NixCo3‐xO4 nanoneedle arrays grown on 3D porous nickel foam (NF) was synthesized as a bifunctional electrocatalyst with OER and HER activity for full water splitting. Benefiting from the advantageous structure, the composite exhibits superior OER activity with an overpotential of 320 mV achieving the current density of 10 mA cm?2. An exceptional HER activity is also acquired with an overpotential of 170 mV at the current density of 10 mA cm?2. Furthermore, the catalyst also shows the superior activity and stability for 20 h when used in the overall water splitting cell. Thus, the hierarchical 3D structure composed of the 1D nanoneedle structure in NixCo3‐xO4/NF represents an avenue to design and develop highly active and bifunctional electrocatalysts for promising energy conversion. 相似文献
2.
Yanmei Shi Yu Yu Yu Liang Yonghua Du Bin Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(12):3809-3813
The oxygen evolution reaction (OER) is an important half reaction in many energy conversion and storage techniques. However, the development of a low‐cost easy‐prepared OER electrocatalyst with high mass activity and rapid kinetics is still challenging. Herein, we report the facile deposition of tannin‐NiFe (TANF) complex film on carbon fiber paper (CP) as a highly efficient OER electrocatalyst. TANF gives rapid OER reaction kinetics with a very small Tafel slope of 28 mV dec?1. The mass activity of TANF reaches 9.17×103 Ag?1 at an overpotential of 300 mV, which is nearly 200‐times larger than that of NiFe double layered hydroxide. Furthermore, tannic acid in TANF can be electrochemically extracted under anodic potential, leaving the inorganic composite NixFe1?xOyHz as the OER‐active species. This work may provide a guide to probing the electrochemical transformation and investigating the reactive species of other metal–organic complexes as heterogeneous electrocatalysts. 相似文献
3.
Strong‐Coupled Cobalt Borate Nanosheets/Graphene Hybrid as Electrocatalyst for Water Oxidation Under Both Alkaline and Neutral Conditions
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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
4.
Nanoscale Trimetallic Metal–Organic Frameworks Enable Efficient Oxygen Evolution Electrocatalysis
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Fei‐Long Li Qi Shao Prof. Xiaoqing Huang Prof. Jian‐Ping Lang 《Angewandte Chemie (International ed. in English)》2018,57(7):1888-1892
Metal–organic frameworks (MOFs) are a class of promising materials for diverse heterogeneous catalysis, but they are usually not directly employed for oxygen evolution electrocatalysis. Most reports focus on using MOFs as templates to in situ create efficient electrocatalysts through annealing. Herein, we prepared a series of Fe/Ni‐based trimetallic MOFs (Fe/Ni/Co(Mn)‐MIL‐53 accordingly to the Material of Institute Lavoisier) by solvothermal synthesis, which can be directly adopted as highly efficient electrocatalysts. The Fe/Ni/Co(Mn)‐MIL‐53 shows a volcano‐type oxygen evolution reaction (OER) activity as a function of compositions. The optimized Fe/Ni2.4/Co0.4‐MIL‐53 can reach a current density of 20 mA cm?2 at low overpotential of 236 mV with a small Tafel slope of 52.2 mV dec?1. In addition, the OER performance of these MOFs can be further enhanced by directly being grown on nickel foam (NF). 相似文献
5.
Mengting Lu Xigaogang Yang Yuwen Li Zhenwang Zhu Yuhang Wu Hui Xu Junkuo Gao Juming Yao 《化学:亚洲杂志》2019,14(19):3357-3362
The preparation of noble metal‐free catalysts for water splitting is the key to low‐cost, sustainable hydrogen generation. Herein, through a pyrolysis‐oxidation process, we prepared a series of Co‐Fe‐Ni trimetallic oxidized carbon nanocubes (Co1‐XFeXNi‐OCNC) with a continuously changeable Co/Fe ratio (X=0, 0.1, 0.2, 0.5, 0.8, 0.9, 1). The Co1‐XFeXNi‐OCNC shows a volcano‐type oxygen evolution reaction (OER) activity. The optimized Co0.1Fe0.9Ni‐OCNC achieves a low overpotential of 268 mV at 10 mA cm?2 with a very low Tafel slope of 48 mV dec?1 in 1 m KOH. At the same time, the stability of the Co0.1Fe0.9Ni‐OCNC is also outstanding; after 1000 CV cycles, the LSV plot is almost coincident. Moreover, the potential remains almost of the same value at 10 mA cm?2 after 12 h in comparison to the initial value. The excellent electrocatalytic properties can be attributed to the synergistic cooperation between each component. Therefore, the Co0.1Fe0.9Ni‐OCNC is a promising candidate instead of precious metal‐based electrocatalysts for OER. 相似文献
6.
Jiaxin Wang Xiaoliang Sun Hanbin Hu Tianyang Shen Guihao Liu Zewei Li Dr. Dongwei Cao Dr. Lei He Prof. Dr. Yu-Fei Song 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(6):e202103601
The low-cost, high-abundance and durable layered double hydroxides (LDHs) have been considered as promising electrocatalysts for oxygen evolution reaction (OER). However, the easy agglomeration of lamellar LDHs in the aqueous phase limits their practical applications. Herein, a series of ternary NiCoFe LDHs were successfully fabricated on nickel foam (NF) via a simple electrodeposition method. The as-prepared Ni(Co0.5Fe0.5)/NF displayed an unique nanoarray structural feature. It showed an OER overpotential of 209 mV at a current density of 10 mA cm−2 in alkaline solution, which was superior to most systems reported so far. As evidenced by the XPS and XAFS results, such excellent performance of Ni(Co0.5Fe0.5)/NF was attributed to the higher Co3+/Co2+ ratio and more defects exposed, comparing with Ni(Co0.5Fe0.5)-bulk and Ni(Co0.5Fe0.5)-mono LDHs prepared by conventional coprecipitation method. Furthermore, the ratio of Co to Fe could significantly tune the Co electronic structure of Ni(CoxFe1-x)/NF composites (x=0.25, 0.50 and 0.75) and affect the electrocatalytic activity for OER, in which Ni(Co0.5Fe0.5)/NF showed the lowest energy barrier for OER rate-determining step (from O* to OOH*). This work proposes a facile method to develop high-efficiency OER electrocatalysts. 相似文献
7.
Jianwen Huang Yaoyao Li Yadong Zhang Gaofeng Rao Chunyang Wu Yin Hu Xianfu Wang Ruifeng Lu Yanrong Li Jie Xiong 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(48):17619-17625
The oxygen evolution reaction (OER) has been explored extensively for reliable hydrogen supply to boost the energy conversion efficiency. The superior OER performance of newly developed non‐noble metal electrocatalysts has concealed the identification of the real active species of the catalysts. Now, the critical active phase in nickel‐based materials (represented by NiNPS) was directly identified by observing the dynamic surface reconstruction during the harsh OER process via combining in situ Raman tracking and ex situ microscopy and spectroscopy analyses. The irreversible phase transformation from NiNPS to α‐Ni(OH)2 and reversible phase transition between α‐Ni(OH)2 and γ‐NiOOH prior to OER demonstrate γ‐NiOOH as the key active species for OER. The hybrid catalyst exhibits 48‐fold enhanced catalytic current at 300 mV and remarkably reduced Tafel slope to 46 mV dec?1, indicating the greatly accelerated catalytic kinetics after surface evolution. 相似文献
8.
A Permselective CeOx Coating To Improve the Stability of Oxygen Evolution Electrocatalysts
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Keisuke Obata Prof. Kazuhiro Takanabe 《Angewandte Chemie (International ed. in English)》2018,57(6):1616-1620
Highly active NiFeOx electrocatalysts for the oxygen evolution reaction (OER) suffer gradual deactivation with time owing to the loss of Fe species from the active sites into solution during catalysis. The anodic deposition of a CeOx layer prevents the loss of such Fe species from the OER catalysts, achieving a highly stable performance. The CeOx layer does not affect the OER activity of the catalyst underneath but exhibits unique permselectivity, allowing the permeation of OH? and O2 through while preventing the diffusion of redox ions through the layer to function as a selective O2‐evolving electrode. The use of such a permselective protective layer provides a new strategy for improving the durability of electrocatalysts. 相似文献
9.
Fei‐Long Li Pengtang Wang Xiaoqing Huang David James Young Hui‐Fang Wang Pierre Braunstein Jian‐Ping Lang 《Angewandte Chemie (International ed. in English)》2019,58(21):7051-7056
Ultrathin metal–organic framework (MOF) nanosheets (NSs) offer potential for many applications, but the synthetic strategies are largely limited to top‐down, low‐yield exfoliation methods. Herein, Ni–M–MOF (M=Fe, Al, Co, Mn, Zn, and Cd) NSs are reported with a thickness of only several atomic layers, prepared by a large‐scale, bottom‐up solvothermal method. The solvent mixture of N,N‐dimethylacetamide and water plays key role in controlling the formation of these two‐dimensional MOF NSs. The MOF NSs can be directly used as efficient electrocatalysts for the oxygen evolution reaction, in which the Ni–Fe–MOF NSs deliver a current density of 10 mA cm?2 at a low overpotential of 221 mV with a small Tafel slope of 56.0 mV dec?1, and exhibit excellent stability for at least 20 h without obvious activity decay. Density functional theory calculations on the energy barriers for OER occurring at different metal sites confirm that Fe is the active site for OER at Ni–Fe–MOF NSs. 相似文献
10.
Yuwen Li Mengting Lu Panpan He Yuhang Wu Jiawen Wang Danni Chen Hui Xu Junkuo Gao Juming Yao 《化学:亚洲杂志》2019,14(9):1590-1594
Non‐noble metal‐based metal–organic framework (MOF)‐derived electrocatalysts have recently attracted great interest in the oxygen evolution reaction (OER). Here we report a facile synthesis of nickel‐based bimetallic electrocatalysts derived from 2D nanosheet‐assembled nanoflower‐like MOFs. The optimized morphologies and large Brunauer–Emmett–Teller (BET) surface area endow FeNi@CNF with efficient OER performance, where the aligned nanosheets can expose abundant active sites and benefit electron transfer. The complex nanoflower morphologies together with the synergistic effects between two metals attributed to the OER activity of the Ni‐based bimetallic catalysts. The optimized FeNi@CNF afforded an overpotential of 356 mV at a current density of 10 mA cm?2 with a Tafel slope of 62.6 mV dec?1, and also exhibited superior durability with only slightly degradation after 24 hours of continuous operation. The results may inspire the use of complex nanosheet‐assembled nanostructures to explore highly active catalysts for various applications. 相似文献
11.
Wei Zhou Dan‐Dan Huang Ya‐Pan Wu Jun Zhao Tao Wu Jian Zhang Dong‐Sheng Li Chenghua Sun Pingyun Feng Xianhui Bu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(13):4271-4275
The integration of heterometallic units and nanostructures into metal–organic frameworks (MOFs) used for the oxygen evolution reaction (OER) can enhance the electrocatalytic performance and help elucidate underlying mechanisms. We have synthesized a series of stable MOFs (CTGU‐10a1–d1) based on trinuclear metal carboxylate clusters and a hexadentate carboxylate ligand with a (6,6)‐connected nia net. We also present a strategy to synthesize hierarchical bimetallic MOF nanostructures (CTGU‐10a2–d2). Among these, CTGU‐10c2 is the best material for the OER, with an overpotential of 240 mV at a current density of 10 mA cm?2 and a Tafel slope of 58 mV dec?1. This is superior to RuO2 and confirms CTGU‐10c2 as one of the few known high‐performing pure‐phase MOF‐OER electrocatalysts. Notably, bimetallic CTGU‐10b2 and c2 show an improved OER activity over monometallic CTGU‐10a2 and d2. Both DFT and experiments show that the remarkable OER performance of CTGU‐10c2 is due to the presence of unsaturated metal sites, a hierarchical nanobelt architecture, and the Ni–Co coupling effect. 相似文献
12.
Fei‐Long Li Pengtang Wang Xiaoqing Huang David James Young Hui‐Fang Wang Pierre Braunstein Jian‐Ping Lang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(21):7125-7130
Ultrathin metal–organic framework (MOF) nanosheets (NSs) offer potential for many applications, but the synthetic strategies are largely limited to top‐down, low‐yield exfoliation methods. Herein, Ni–M–MOF (M=Fe, Al, Co, Mn, Zn, and Cd) NSs are reported with a thickness of only several atomic layers, prepared by a large‐scale, bottom‐up solvothermal method. The solvent mixture of N,N‐dimethylacetamide and water plays key role in controlling the formation of these two‐dimensional MOF NSs. The MOF NSs can be directly used as efficient electrocatalysts for the oxygen evolution reaction, in which the Ni–Fe–MOF NSs deliver a current density of 10 mA cm?2 at a low overpotential of 221 mV with a small Tafel slope of 56.0 mV dec?1, and exhibit excellent stability for at least 20 h without obvious activity decay. Density functional theory calculations on the energy barriers for OER occurring at different metal sites confirm that Fe is the active site for OER at Ni–Fe–MOF NSs. 相似文献
13.
Sheng Yang Guangbo Chen Antonio Gaetano Ricciardulli Panpan Zhang Zhen Zhang Huanhuan Shi Ji Ma Jian Zhang Paul W. M. Blom Xinliang Feng 《Angewandte Chemie (International ed. in English)》2020,59(1):465-470
Transition‐metal phosphides (TMPs) have emerged as a fascinating class of narrow‐gap semiconductors and electrocatalysts. However, they are intrinsic nonlayered materials that cannot be delaminated into two‐dimensional (2D) sheets. Here, we demonstrate a general bottom‐up topochemical strategy to synthesize a series of 2D TMPs (e.g. Co2P, Ni12P5, and CoxFe2?xP) by using phosphorene sheets as the phosphorus precursors and 2D templates. Notably, 2D Co2P is a p‐type semiconductor, with a hole mobility of 20.8 cm2 V?1 s?1 at 300 K in field‐effect transistors. It also behaves as a promising electrocatalyst for the oxygen evolution reaction (OER), thanks to the charge‐transport modulation and improved surface exposure. In particular, iron‐doped Co2P (i.e. Co1.5Fe0.5P) delivers a low overpotential of only 278 mV at a current density of 10 mA cm?2 that outperforms the commercial Ir/C benchmark (304 mV). 相似文献
14.
Rahul Majee Arun Kumar Tisita Das Sudip Chakraborty Sayan Bhattacharyya 《Angewandte Chemie (International ed. in English)》2020,59(7):2881-2889
Five‐fold intertwined AgxNi1?x (x=0.01–0.25) heterogeneous alloy nanocrystal (NC) catalysts, prepared through unique reagent combinations, are presented. With only ca. 5 at % Ag (AgNi‐5), Pt‐like activity has been achieved at pH 14. To reach a current density of 10 mA cm?2 the extremely stable AgNi‐5 requires an overpotential of 24.0±1.2 mV as compared to 20.1±0.8 mV for 20 % Pt/C, both with equal catalyst loading of 1.32 mg cm?2. The turnover frequency (TOF) is as high as 2.1 H2 s?1 at 50 mV (vs. RHE). Site‐specific elemental analyses show the Ag:Ni compositional variation, where the apex and edges of the decahedra are Ag‐rich, thereby exposing Ni onto the faces to achieve maximum charge transport for an exceptional pH universal HER activity. DFT calculations elucidate the relative H‐atom adsorption capability of the Ni centers as a function of their proximity to Ag atom. 相似文献
15.
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
16.
Linzhou Zhuang Yi Jia Hongli Liu Zhiheng Li Mengran Li Longzhou Zhang Xin Wang Dongjiang Yang Zhonghua Zhu Xiangdong Yao 《Angewandte Chemie (International ed. in English)》2020,59(34):14664-14670
The oxygen vacancies of defective iron–cobalt oxide (FeCoOx‐Vo) nanosheets are modified by the homogeneously distributed sulfur (S) atoms. S atoms can not only effectively stabilize oxygen vacancies (Vo), but also form the Co?S coordination with Co active site in the Vo, which can modulate the electronic structure of the active site, enabling FeCoOx‐Vo‐S to exhibit much superior OER activity. FeCoOx‐Vo‐S exhibits a mass activity of 2440.0 A g?1 at 1.5 V vs. RHE in 1.0 m KOH, 25.4 times higher than that of RuO2. The Tafel slope is as low as 21.0 mV dec?1, indicative of its excellent charge transfer rate. When FeCoOx‐Vo‐S (anode catalyst) is paired with the defective CoP3/Ni2P (cathode catalyst) for overall water splitting, current densities of as high as 249.0 mA cm?2 and 406.0 mA cm?2 at a cell voltage of 2.0 V and 2.3 V, respectively, can be achieved. 相似文献
17.
Hongbo Yu Lixia Wang Huatong Li Zuyang Luo Dr. Tayirjan Taylor Isimjan Prof. Dr. Xiulin Yang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(60):e202201784
Metal-organic frameworks (MOFs) have been considered as potential oxygen evolution reaction (OER) electrocatalysts owning to their ultra-thin structure, adjustable composition, high surface area, and high porosity. Here, we designed and fabricated a vanadium-doped nickel organic framework (V1−x−NixMOF) system by using a facile two-step solvothermal method on nickel foam (NF). The doping of vanadium remarkably elevates the OER activity of V1−x−NixMOF, thus demonstrating better performance than the corresponding single metallic Ni-MOF, NiV-MOF and RuO2 catalysts at high current density (>400 mA cm−2). V0.09−Ni0.91MOF/NF provides a low overpotential of 235 mV and a small Tafel slope of 30.3 mV dec−1 at a current density of 10 mA cm−2. More importantly, a water-splitting device assembled with Pt/C/NF and V0.09−Ni0.91MOF/NF as cathode and anode yielded a cell voltage of 1.96 V@1000 mA cm−2, thereby outperforming the-state-of-the-art RuO2(+)||Pt/C(−). Our work sheds new insight on preparing stable, efficient OER electrocatalysts and a promising method for designing various MOF-based materials. 相似文献
18.
《化学:亚洲杂志》2017,12(20):2720-2726
Iron‐based (oxy)hydroxides are especially attractive electrocatalysts for the oxygen evolution reaction (OER) owing to their earth abundance, low cost, and nontoxicity. However, poor OER kinetics on the surface restricts the performance of the FeOOH electrocatalyst. Herein, a highly efficient and stable Ni(OH)2/β‐like FeOOH electrocatalyst is obtained by facile electroactivation treatment. The activated Ni(OH)2/β‐like FeOOH sample indicates an overpotential of 300 mV at 10 mA cm−2 for the OER, and no clear current decay after 50 h of testing; this is comparable to the most efficient nickel‐ and cobalt‐based electrocatalysts on planar substrates. Furthermore, studies suggest that β‐like FeOOH plays a key role in remarkably enhancing the performance during the electroactivation process owing to its metastable tunnel structure with a lower barrier for interface diffusion of Ni2+ ions between the bilayer electrocatalyst. This study develops a new strategy to explore efficient and low‐cost electrocatalysts and deepens understanding of bilayer electrocatalysts for the OER. 相似文献
19.
Exploring advanced electrocatalysts for electrocatalytic hydrogen evolution is highly desired but remains a challenge due to the lack of an efficient preparation method and reasonable structural design. Herein, we deliberately designed novel Ag/WO3?x heterostructures through a supercritical CO2‐assisted exfoliation‐oxidation route and the subsequent loading of Ag nanoparticles. The ultrathin and oxygen vacancies‐enriched WO3?x nanosheets are ideal substrates for loading Ag nanoparticles, which can largely increase the active site density and improve electron transport. Besides, the resultant WO3?x nanosheets with porous structure can form during the electrochemical cycling process induced by an electric field. As a result, the exquisite Ag/WO3?x heterostructures show an enhanced hydrogen evolution reaction (HER) activity with a low onset overpotential of ≈30 mV, a small Tafel slope of ≈40 mV dec?1 at 10 mA cm?2, and as well as long‐term durability. This work sheds light on material design and preparation, and even opens up an avenue for the development of high‐efficiency electrocatalysts. 相似文献
20.
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