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1.
Integrating NiCo Alloys with Their Oxides as Efficient Bifunctional Cathode Catalysts for Rechargeable Zinc–Air Batteries
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Dr. Xien Liu Minjoon Park Dr. Min Gyu Kim Shiva Gupta Prof. Gang Wu Prof. Jaephil Cho 《Angewandte Chemie (International ed. in English)》2015,54(33):9654-9658
The lack of high‐efficient, low‐cost, and durable bifunctional electrocatalysts that act simultaneously for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is currently one of the major obstacles to commercializing the electrical rechargeability of zinc–air batteries. A nanocomposite CoO‐NiO‐NiCo bifunctional electrocatalyst supported by nitrogen‐doped multiwall carbon nanotubes (NCNT/CoO‐NiO‐NiCo) exhibits excellent activity and stability for the ORR/OER in alkaline media. More importantly, real air cathodes made from the bifunctional NCNT/CoO‐NiO‐NiCo catalysts further demonstrated superior performance to state‐of‐the‐art Pt/C or Pt/C+IrO2 catalysts in primary and rechargeable zinc–air batteries. 相似文献
2.
Exploring the Performance Improvement of the Oxygen Evolution Reaction in a Stable Bimetal–Organic Framework System
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Xiao‐Li Wang Long‐Zhang Dong Man Qiao Yu‐Jia Tang Dr. Jiang Liu Prof. Yafei Li Prof. Shun‐Li Li Jia‐Xin Su Prof. Ya‐Qian Lan 《Angewandte Chemie (International ed. in English)》2018,57(31):9660-9664
Despite wide applications of bimetallic electrocatalysis in oxygen evolution reaction (OER) owing to their superior performance, the origin of the improved performance remains elusive. The underlying mechanism was explored by designing and synthesizing a series of stable metal–organic frameworks (MOFs: NNU‐21–24 ) based on trinuclear metal carboxylate clusters and tridentate carboxylate ligands. Among the examined stable MOFs, NNU‐23 exhibits the best OER performance; particularly, compared with monometallic MOFs, all the bimetallic MOFs display improved OER activity. DFT calculations and experimental results demonstrate that introduction of the second metal atom can improve the activity of the original atom. The proposed model of bimetallic electrocatalysts affecting their OER performance can facilitate design of efficient bimetallic catalysts for energy storage and conversion, and investigation of the related catalytic mechanisms. 相似文献
3.
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
4.
Synthesis of Nanoporous Carbon–Cobalt‐Oxide Hybrid Electrocatalysts by Thermal Conversion of Metal–Organic Frameworks
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Dr. Watcharop Chaikittisilp Dr. Nagy L. Torad Dr. Cuiling Li Dr. Masataka Imura Dr. Norihiro Suzuki Dr. Shinsuke Ishihara Prof. Dr. Katsuhiko Ariga Prof. Dr. Yusuke Yamauchi 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(15):4217-4221
Nanoporous carbon–cobalt‐oxide hybrid materials are prepared by a simple, two‐step, thermal conversion of a cobalt‐based metal–organic framework (zeolitic imidazolate framework‐9, ZIF‐9). ZIF‐9 is carbonized in an inert atmosphere to form nanoporous carbon–metallic‐cobalt materials, followed by the subsequent thermal oxidation in air, yielding nanoporous carbon–cobalt‐oxide hybrids. The resulting hybrid materials are evaluated as electrocatalysts for the oxygen‐reduction reaction (ORR) and the oxygen‐evolution reaction (OER) in a KOH electrolyte solution. The hybrid materials exhibit similar catalytic activity in the ORR to the benchmark, commercial, Pt/carbon black catalyst, and show better catalytic activity for the OER than the Pt‐based catalyst. 相似文献
5.
Weijin Li Song Xue Sebastian Watzele Shujin Hou Johannes Fichtner A. Lisa Semrau Liujiang Zhou Alexander Welle Aliaksandr S. Bandarenka Roland A. Fischer 《Angewandte Chemie (International ed. in English)》2020,59(14):5837-5843
Metal–organic frameworks (MOFs) and their derivatives are considered as promising catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), which are important for many energy provision technologies, such as electrolyzers, fuel cells and some types of advanced batteries. In this work, a “strain modulation” approach has been applied through the use of surface‐mounted NiFe‐MOFs in order to design an advanced bifunctional ORR/OER electrocatalyst. The material exhibits an excellent OER activity in alkaline media, reaching an industrially relevant current density of 200 mA cm?2 at an overpotential of only ≈210 mV. It demonstrates operational long‐term stability even at a high current density of 500 mA cm?2 and exhibits the so far narrowest “overpotential window” ΔEORR‐OER of 0.69 V in 0.1 m KOH with a mass loading being two orders of magnitude lower than that of benchmark electrocatalysts. 相似文献
6.
Li An Bolong Huang Yu Zhang Rui Wang Nan Zhang Tengyuan Dai Pinxian Xi Chun‐Hua Yan 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(28):9559-9563
Atomic‐thick interfacial dominated bifunctional catalyst NiO/CoO transition interfacial nanowires (TINWs) with abundant defect sites display high electroactivity and durability in the oxygen evolution reaction (OER) and the oxygen reduction reaction (ORR). Density functional theory (DFT) calculations show that the excellent OER/ORR performance arises from the electron‐rich interfacial region coupled with defect sites, thus enabling a fast‐redox rate with lower activation barrier for fast electron transfer. When assembled as an air‐electrode, NiO/CoO TINWs delivered the high specific capacity of 842.58 mAh gZn?1, the large energy density of 996.44 Wh kgZn?1 with long‐time stability of more than 33 h (25 °C), and superior performance at low (?10 °C) and high temperature (80 °C). 相似文献
7.
Pomegranate‐Inspired Design of Highly Active and Durable Bifunctional Electrocatalysts for Rechargeable Metal–Air Batteries
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Dr. Ge Li Dr. Xiaolei Wang Jing Fu Dr. Jingde Li Moon Gyu Park Dr. Yining Zhang Gregory Lui Prof. Zhongwei Chen 《Angewandte Chemie (International ed. in English)》2016,55(16):4977-4982
Rational design of highly active and durable electrocatalysts for oxygen reactions is critical for rechargeable metal–air batteries. Herein, we report the design and development of composite electrocatalysts based on transition metal oxide nanocrystals embedded in a nitrogen‐doped, partially graphitized carbon framework. Benefiting from the unique pomegranate‐like architecture, the composite catalysts possess abundant active sites, strong synergetic coupling, enhanced electron transfer, and high efficiencies in the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). The Co3O4‐based composite electrocatalyst exhibited a high half‐wave potential of 0.842 V for ORR, and a low overpotential of only 450 mV at the current density of 10 mA cm?2 for OER. A single‐cell zinc–air battery was also fabricated with superior durability, holding great promise in the practical implementation of rechargeable metal–air batteries. 相似文献
8.
Fangyi Cheng Qing Zhao Xiaopeng Han Jun Chen 《Angewandte Chemie (International ed. in English)》2015,54(14):4338-4343
The ever‐increasing consumption of a huge quantity of lithium batteries, for example, Li–MnO2 cells, raises critical concern about their recycling. We demonstrate herein that decayed Li–MnO2 cells can be further utilized as rechargeable lithium–air cells with admitted oxygen. We further investigated the effects of lithiated manganese dioxide on the electrocatalytic properties of oxygen‐reduction and oxygen‐evolution reactions (ORR/OER). The catalytic activity was found to be correlated with the composition of LixMnO2 electrodes (0<x<1) generated in situ in aprotic Li–MnO2 cells owing to tuning of the Mn valence and electronic structure. In particular, modestly lithiated Li0.50MnO2 exhibited superior performance with enhanced round‐trip efficiency (ca. 76 %), high cycling ability (190 cycles), and high discharge capacity (10 823 mA h gcarbon?1). The results indicate that the use of depleted Li–MnO2 batteries can be prolonged by their application as rechargeable lithium–air batteries. 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.
Nitrogen,Phosphorus, and Fluorine Tri‐doped Graphene as a Multifunctional Catalyst for Self‐Powered Electrochemical Water Splitting
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Dr. Jintao Zhang Prof. Liming Dai 《Angewandte Chemie (International ed. in English)》2016,55(42):13296-13300
Electrocatalysts are required for clean energy technologies (for example, water‐splitting and metal‐air batteries). The development of a multifunctional electrocatalyst composed of nitrogen, phosphorus, and fluorine tri‐doped graphene is reported, which was obtained by thermal activation of a mixture of polyaniline‐coated graphene oxide and ammonium hexafluorophosphate (AHF). It was found that thermal decomposition of AHF provides nitrogen, phosphorus, and fluorine sources for tri‐doping with N, P, and F, and simultaneously facilitates template‐free formation of porous structures as a result of thermal gas evolution. The resultant N, P, and F tri‐doped graphene exhibited excellent electrocatalytic activities for the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). The trifunctional metal‐free catalyst was further used as an OER–HER bifunctional catalyst for oxygen and hydrogen gas production in an electrochemical water‐splitting unit, which was powered by an integrated Zn–air battery based on an air electrode made from the same electrocatalyst for ORR. The integrated unit, fabricated from the newly developed N, P, and F tri‐doped graphene multifunctional metal‐free catalyst, can operate in ambient air with a high gas production rate of 0.496 and 0.254 μL s?1 for hydrogen and oxygen gas, respectively, showing great potential for practical applications. 相似文献
12.
《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
13.
Dongfeng Du Shuo Zhao Zhuo Zhu Fujun Li Jun Chen 《Angewandte Chemie (International ed. in English)》2020,59(41):18140-18144
The storage of solar energy in battery systems is pivotal for a sustainable society, which faces many challenges. Herein, a Zn–air battery is constructed with two cathodes of poly(1,4‐di(2‐thienyl))benzene (PDTB) and TiO2 grown on carbon papers to sandwich a Zn anode. The PDTB cathode is illuminated in a discharging process, in which photoelectrons are excited into the conduction band of PDTB to promote oxygen reduction reaction (ORR) and raise the output voltage. In a reverse process, holes in the valence band of the illuminated TiO2 cathode are driven for the oxygen evolution reaction (OER) by an applied voltage. A record‐high discharge voltage of 1.90 V and an unprecedented low charge voltage of 0.59 V are achieved in the photo‐involved Zn–air battery, regardless of the equilibrium voltage. This work offers an innovative pathway for photo‐energy utilization in rechargeable batteries. 相似文献
14.
Jiayue Tian Feilong Jiang Daqiang Yuan Linjie Zhang Qihui Chen Maochun Hong 《Angewandte Chemie (International ed. in English)》2020,59(31):13101-13108
Facile preparation of low‐cost electrocatalysts for efficient oxygen evolution reaction (OER) remains a big challenge. Herein, a novel strategy for ultrafast (20 s) transformation of bulk metal–organic frameworks (MOFs) into ultrathin metal oxyhydroxide nanosheets for efficient OER has been developed. For two isomeric MOFs ( FJI‐H25Fe and FJI‐H25FeCo ), only the metastable FJI‐H25FeCo bulk can immediately transform into FeCo‐oxyhydroxides nanosheets through electric‐field assisted hydrolysis. The potential evolution process from MOF bulk to FeCo‐oxyhydroxides nanosheets has been investigated in detail. The as‐made nanosheets exhibit excellent OER performances, showing an extremely low overpotential of 231 mV at the current density of 10 mA cm?2, a relatively small Tafel slope of 42 mV dec?1, and long‐term durability of at least 30 h. This work not only provides a novel strategy for facile preparation of low‐cost and efficient OER electrocatalysts, but also represents a new way for preparation of metal oxyhydroxides nanosheets with good crystallinity and morphology, and a fresh method for mild synthesis of nanosized derivatives from MOF materials. 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.
Weiren Cheng Xue Feng Lu Deyan Luan Xiong Wen Lou 《Angewandte Chemie (International ed. in English)》2020,59(41):18234-18239
Developing noble‐metal‐free bifunctional oxygen electrocatalysts is of great significance for energy conversion and storage systems. Herein, we have developed a transformation method for growing NiMn‐based bimetal–organic framework (NiMn‐MOF) nanosheets on multi‐channel carbon fibers (MCCF) as a bifunctional oxygen electrocatalyst. Owing to the desired components and architecture, the MCCF/NiMn‐MOFs manifest comparable electrocatalytic performance towards oxygen reduction reaction (ORR) with the commercial Pt/C electrocatalyst and superior performance towards oxygen evolution reaction (OER) to the benchmark RuO2 electrocatalyst. X‐ray absorption fine structure (XAFS) spectroscopy and density functional theory (DFT) calculations reveal that the strong synergetic effect of adjacent Ni and Mn nodes within MCCF/NiMn‐MOFs effectively promotes the thermodynamic formation of key *O and *OOH intermediates over active NiO6 centers towards fast ORR and OER kinetics. 相似文献
17.
Activity and Stability of Ruddlesden–Popper‐Type Lan+1NinO3n+1 (n=1, 2, 3, and ∞) Electrocatalysts for Oxygen Reduction and Evolution Reactions in Alkaline Media
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Jie Yu Dr. Jaka Sunarso Yinlong Zhu Xiaomin Xu Prof. Ran Ran Prof. Wei Zhou Prof. Zongping Shao 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(8):2719-2727
Increasing energy demands have stimulated intense research activity on cleaner energy conversion such as regenerative fuel cells and reversible metal–air batteries. It is highly challenging but desirable to develop low‐cost bifunctional catalysts for both the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER), the lack of which is currently one of the major limiting components towards commercialization of these technologies. Here, we have conducted a systematic study on the OER and ORR performances of the Ruddlesden–Popper family of Lan+1NinO3n+1 (n=1, 2, 3, and ∞) in an alkaline medium for the first time. It is apparent that the Ni?O bond lengths and the hyperstoichiometric oxides in the rock‐salt layers correlate with the ORR activities, whereas the OER activities appear to be influenced by the OH? content on the surface of the compounds. In our case, the electronic configuration fails to predict the electrocatalytic activity of these compounds. This work provides guidelines to develop new electrocatalysts with improved performances. 相似文献
18.
Hydrothermal Synthesis of Metal–Polyphenol Coordination Crystals and Their Derived Metal/N‐doped Carbon Composites for Oxygen Electrocatalysis
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Dr. Jing Wei Yan Liang Yaoxin Hu Dr. Biao Kong Jin Zhang Dr. Qinfen Gu Dr. Yuping Tong Dr. Xianbiao Wang Prof. San Ping Jiang Prof. Huanting Wang 《Angewandte Chemie (International ed. in English)》2016,55(40):12470-12474
Cobalt (or iron)–polyphenol coordination polymers with crystalline frameworks are synthesized for the first time. The crystalline framework is formed by the assembly of metal ions and polyphenol followed by oxidative self‐polymerization of the organic ligands (polyphenol) during hydrothermal treatment in alkaline condition. As a result, such coordination crystals are even partly stable in strong acid (such as 2 m HCl). The metal (Co or Fe)‐natural abundant polyphenol (tannin) coordination crystals are a renewable source for the fabrication of metal/carbon composites as a nonprecious‐metal catalyst, which show high catalytic performance for both oxygen reduction reaction and oxygen evolution reaction. Such excellent performance makes metal–polyphenol coordination crystals an efficient precursor to fabricate low‐cost catalysts for the large‐scale application of fuel cells and metal–air batteries. 相似文献
19.
Core–Shell NiO@Ni‐P Hybrid Nanosheet Array for Synergistically Enhanced Oxygen Evolution Electrocatalysis: Experimental and Theoretical Insights
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Shuai Hao Ninghua Chen Qin Liu Prof. Ying Xie Prof. Honggang Fu Prof. Yingchun Yang 《化学:亚洲杂志》2018,13(8):944-949
Cost‐effective and highly‐efficient electrocatalysts for the oxygen evolution reaction are crucial for electrolytic hydrogen production. Here, we report core–shell NiO@Ni‐P nanosheet arrays as a high‐performance 3D catalyst for water oxidation electrocatalysis. Such nanoarrays demand overpotentials of 292 and 350 mV to drive geometrical catalytic current densities of 10 and 100 mA cm?2, respectively, with an activity superior to its NiO and Ni‐P counterparts. Notably, this catalyst also shows a high long‐term electrochemical durability with a Faradaic efficiency of 98.1 %. Density functional theory calculation reveals that the superior activity benefits from the synergistic effect between NiO and Ni‐P. 相似文献
20.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(14):3955-3958
Hollow nanostructures have attracted increasing research interest in electrochemical energy storage and conversion owing to their unique structural features. However, the synthesis of hollow nanostructured metal phosphides, especially nonspherical hollow nanostructures, is rarely reported. Herein, we develop a metal–organic framework (MOF)‐based strategy to synthesize carbon incorporated Ni–Co mixed metal phosphide nanoboxes (denoted as NiCoP/C). The oxygen evolution reaction (OER) is selected as a demonstration to investigate the electrochemical performance of the NiCoP/C nanoboxes. For comparison, Ni–Co layered double hydroxide (Ni–Co LDH) and Ni–Co mixed metal phosphide (denoted as NiCoP) nanoboxes have also been synthesized. Benefiting from their structural and compositional merits, the as‐synthesized NiCoP/C nanoboxes exhibit excellent electrocatalytic activity and long‐term stability for OER. 相似文献