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1.
Qing Dong Hui Wang Prof. Shan Ji Xuyun Wang Prof. Zaiyong Mo Prof. Vladimir Linkov Prof. Rongfang Wang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(47):10752-10758
Cost efficient bifunctional air cathodes possessing high electrocatalytic activity are of great importance for the development of secondary Zn-air batteries. In this work, cobalt nanoparticles are encapsulated within a 3D N-doped open network of carbon tubes (Co@N-CNTs) by a molten-salt synthesis procedure conducted at a high temperature. Physical characterization demonstrates that Co@N-CNTs are comprised of Co particle inserted carbon tubes with mesoporous tube walls, providing significant active surface area for electrochemical reactions. High electrocatalytic activity of Co@N-CNTs towards both oxygen evolution and oxygen reduction reactions is due to its well-developed active surface and a synergistic effect between N-doped carbon and Co nanoparticles. Both primary and secondary Zn-air battery cells assembled using Co@N-CNTs as an air cathode show higher electrochemical performance than similar cells containing commercial Pt/C and Pt/C +RuO2, making the newly developed material a promising alternative to existing metal-based air cathodes. 相似文献
2.
锌-空气电池因其拥有理想的能量密度和功率密度,并有望在能源转化与储存领域的广泛应用,引起国内外研究者的高度关注. 其中,空气电极作为氧催化反应的核心区域,更是整个锌-空气电池研究的重点. 近年来,非贵金属双功能催化剂及其电极以其高活性、低成本以及种类丰富等特点取得了较多的研究成果. 本文综述了非贵金属氧化物催化剂、碳基催化剂、碳载过渡金属化合物复合材料以及自支撑电极在锌-空气电池中的反应机制和研究进展,提出了高效双功能催化剂的构建策略,并对双功能催化剂/电极的发展趋势进行了展望. 相似文献
3.
Yuanjun Chen Shufang Ji Dr. Yanggang Wang Dr. Juncai Dong Dr. Wenxing Chen Zhi Li Rongan Shen Dr. Lirong Zheng Prof. Zhongbin Zhuang Prof. Dr. Dingsheng Wang Prof. Dr. Yadong Li 《Angewandte Chemie (International ed. in English)》2017,56(24):6937-6941
The development of low-cost, efficient, and stable electrocatalysts for the oxygen reduction reaction (ORR) is desirable but remains a great challenge. Herein, we made a highly reactive and stable isolated single-atom Fe/N-doped porous carbon (ISA Fe/CN) catalyst with Fe loading up to 2.16 wt %. The catalyst showed excellent ORR performance with a half-wave potential (E1/2) of 0.900 V, which outperformed commercial Pt/C and most non-precious-metal catalysts reported to date. Besides exceptionally high kinetic current density (Jk) of 37.83 mV cm−2 at 0.85 V, it also had a good methanol tolerance and outstanding stability. Experiments demonstrated that maintaining the Fe as isolated atoms and incorporating nitrogen was essential to deliver the high performance. First principle calculations further attributed the high reactivity to the high efficiency of the single Fe atoms in transporting electrons to the adsorbed OH species. 相似文献
4.
在金属空气电池和燃料电池阴极上的氧还原反应(ORR)对相关电化学能量转换装置的整体性能有重要影响,金属-氮-碳催化剂有望替代传统的商业Pt-C成为新一代ORR电催化剂。本文通过简便的一步热解工艺合成了具有Fe-Nx活性位点和Fe2O3纳米颗粒共存的电催化剂,Fe2O3@Fe-N-C-1000催化剂在0.1 mol·L-1 KOH溶液中表现出良好的ORR活性,半波电位为0.84 V,应用在锌-空气电池中时也具有可以和商业Pt-C媲美的性能,能量密度为88.3 mW·cm-2,同时和Pt-C相比具有更好电化学稳定性,表现出优良的ORR应用潜力。 相似文献
5.
Haichao Yang Ao Xie Dr. Yang Tang Zixiang Wang Jinpeng Zhang Dr. Lingpo Kong Dr. Peng Song Dr. Yanzhi Sun Dr. Xiaojin Yang Prof. Pingyu Wan 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(2):e202103275
It is a great challenge to fabricate highly efficient pH-universal electrocatalysts for oxygen reduction reaction (ORR). Herein, a facile strategy, which includes coating the Fe modified ZIF8 on Cu foil and in situ pyrolysis to evaporate and dope Cu into the MOF derived carbon, is developed to fabricate Fe/Cu−N co-doped carbon material (Cu/Fe−NC). Profiting from the modulated electron distribution and textual properties, well-designed Cu/Fe−NC exhibits superior half-wave potential (E1/2) of 0.923 V in alkaline, 0.757 V in neutral and comparable 0.801 V in acid electrolytes, respectively. Furthermore, the ultralow peroxides yield of ORR demonstrates the high selectivity of Cu/Fe−NC in full pH scale electrolytes. As expected, the self-made alkaline and neutral zinc-air batteries equipped with Cu/Fe−NC cathode display excellent discharge voltages, outstanding peak power densities and remarkable stability. This work opens a new way to fabricate highly efficient and pH-universal electrocatalysts for ORR through strategy of Fe/Cu−N co-doping, Cu foil evaporation and carbon defects capture. 相似文献
6.
随着金属空气电池技术的不断发展,氧还原催化剂成为限制其动力化的最主要瓶颈之一。近几年来,石墨烯基氧还原催化剂(GORRC)由于优异的氧还原催化活性而备受关注。本文结合石墨烯基氧还原催化剂的研究现状,将其分为三类:石墨烯作氧还原催化剂载体,氮掺杂石墨烯作为氧还原催化剂,以及氮掺杂石墨烯与其他催化剂形成的复合催化体系,并对这三种石墨烯基氧还原催化剂进行了详细的综述。石墨烯作为一种优良的催化剂载体,能够显著降低活性物质负载量,提高氧还原催化剂的催化活性和长期稳定性。氮掺杂石墨烯显示了优良的氧还原催化性能。氮掺杂石墨烯与其他催化剂复合后,由于两者之间的相互作用,可得到性能更为优异的氧还原催化剂。最后,本文还对石墨烯基氧还原催化剂及其在金属空气电池中的研究前景和发展方向进行了展望,指出了将来的研究重点。 相似文献
7.
Efficient Oxygen Reduction Reaction (ORR) Catalysts Based on Single Iron Atoms Dispersed on a Hierarchically Structured Porous Carbon Framework
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Dr. Zhengping Zhang Dr. Junting Sun Prof. Feng Wang Prof. Liming Dai 《Angewandte Chemie (International ed. in English)》2018,57(29):9038-9043
Single Fe atoms dispersed on hierarchically structured porous carbon (SA‐Fe‐HPC) frameworks are prepared by pyrolysis of unsubstituted phthalocyanine/iron phthalocyanine complexes confined within micropores of the porous carbon support. The single‐atom Fe catalysts have a well‐defined atomic dispersion of Fe atoms coordinated by N ligands on the 3D hierarchically porous carbon support. These SA‐Fe‐HPC catalysts are comparable to the commercial Pt/C electrode even in acidic electrolytes for oxygen reduction reaction (ORR) in terms of the ORR activity (E1/2=0.81 V), but have better long‐term electrochemical stability (7 mV negative shift after 3000 potential cycles) and fuel selectivity. In alkaline media, the SA‐Fe‐HPC catalysts outperform the commercial Pt/C electrode in ORR activity (E1/2=0.89 V), fuel selectivity, and long‐term stability (1 mV negative shift after 3000 potential cycles). Thus, these nSA‐Fe‐HPCs are promising non‐platinum‐group metal ORR catalysts for fuel‐cell technologies. 相似文献
8.
析氧反应(OER)催化剂在锌空气电池(ZABs)储能过程中起着关键作用。我们开发了一种新型非贵金属基自支撑碳纳米纤维催化剂(NiδFe4-δ-CNF)。首先,以聚乙烯吡咯烷酮、过渡金属乙酸酯、N,N-二甲基甲酰胺为原料,采用静电纺丝法制备了网状前驱体。随后,通过高温退火处理,将其转化为三维(3D)多孔结构材料。合成的Ni1Fe1-CNF催化剂在浓度为1 mol·L-1KOH的电解质溶液中具有较低的起始电位(230 m V)和过电势(280 mV,10 mA·cm-2),性能优于商业RuO2。同时,将Ni1Fe1-CNF催化剂与商业Pt/C催化剂混合,作为空气阴极催化剂组装成ZAB,与商业的RuO2+Pt/C ZAB相比,Ni1Fe1-CNF+Pt/C ZAB具有更高的功率密度(122 m W·cm-2)、... 相似文献
9.
Hao Zhang Wei Xia Haoming Shen Wenhan Guo Zibin Liang Kexin Zhang Yingxiao Wu Bingjun Zhu Ruqiang Zou 《Angewandte Chemie (International ed. in English)》2020,59(5):1871-1877
Antiperovskite Co3InC0.7N0.3 nanomaterials with highly enhanced oxygen reduction reaction (ORR) performance were prepared by tuning nitrogen contents through a metal–organic framework (MOF)‐derived strategy. The nanomaterial surpasses all reported noble‐metal‐free antiperovskites and even most perovskites in terms of onset potential (0.957 V at J=0.1 mA cm?2) and half‐wave potential (0.854 V). The OER and zinc–air battery performance demonstrate its multifunctional oxygen catalytic activities. DFT calculation was performed and for the first time, a 4 e? dissociative ORR pathway on (200) facets of antiperovskite was revealed. Free energy studies showed that nitrogen substitution could strengthen the OH desorption as well as hydrogenation that accounts for the enhanced ORR performance. This work expands the scope for material design via tailoring the nitrogen contents for optimal reaction free energy and hence performance of the antiperovskite system. 相似文献
10.
Kejun Tu Lingyi Zou Dr. Chongqing Yang Prof. Yuezeng Su Chenbao Lu Dr. Jinhui Zhu Prof. Fan Zhang Dr. Changchun Ke Prof. Xiaodong Zhuang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(29):6525-6534
Two-dimensional (2D) porous carbon nanosheets (2DPCs) have attracted great attention for their good porosity and long-distance conductivity. Factors such as templates, precursors, and carbonization–activation methods, directly determine their performance. However, rational design and preparation of porous carbon materials with controlled 2D morphology and heteroatom dopants remains a challenge. Therefore, an ionic polyimide with both sp2- and sp3-hybridized nitrogen atoms was prepared as a precursor for fabricating N-doped hexagonal porous carbon nanosheets through a hard-template approach. Because of the large surface area and efficient charge-mass transport, the resulting activated 2D porous carbon nanosheets (2DPCs-a) displayed promising electrocatalytic properties for oxygen reduction reaction (ORR) in alkaline and acidic media, such as ultralow half-wave potential (0.83 vs. 0.84 V of Pt/C) and superior limiting current density (5.42 vs. 5.14 mA cm−2 of Pt/C). As air cathodes in Zn–air batteries, the as-developed 2DPCs-a exhibited long stability and high capacity (up to 614 mA h g−1), which are both higher than those of commercial Pt/C. This work provides a convenient method for controllable and scalable 2DPCs fabrication as well as new opportunities to develop high-efficiency electrocatalysts for ORR and Zn–air batteries. 相似文献
11.
Shunyao Yan Zixun Yu Chang Liu Ziwen Yuan Chaojun Wang Junsheng Chen Li Wei Yuan Chen 《化学:亚洲杂志》2020,15(12):1881-1889
Cost‐effective and high‐performance electrocatalysts for oxygen reduction reactions (ORR) are needed for many energy storage and conversion devices. Here, we demonstrate that whey powder, a major by‐product in the dairy industry, can be used as a sustainable precursor to produce heteroatom doped carbon electrocatalysts for ORR. Rich N and S compounds in whey powders can generate abundant catalytic active sites. However, these sites are not easily accessible by reactants of ORR. A dual‐template method was used to create a hierarchically and interconnected porous structure with micropores created by ZnCl2 and large mesopores generated by fumed SiO2 particles. At the optimum mass ratio of whey power: ZnCl2 : SiO2 at 1 : 3 : 0.8, the resulting carbon material has a large specific surface area close to 2000 m2 g?1, containing 4.6 at.% of N with 39.7% as pyridinic N. This carbon material shows superior electrocatalytic activity for ORR, with an electron transfer number of 3.88 and a large kinetic limiting current density of 45.40 mA cm?2. They were employed as ORR catalysts to assemble primary zinc‐air batteries, which deliver a power density of 84.1 mW cm?2 and a specific capacity of 779.5 mAh g?1, outperforming batteries constructed using a commercial Pt/C catalyst. Our findings open new opportunities to use an abundant biomaterial, whey powder, to create high‐value‐added carbon electrocatalysts for emerging energy applications. 相似文献
12.
Bifunctional electrocatalysts play a key role in the performance of rechargeable metal-air batteries. Herein, we report a hybrid catalyst, Ag1.8Mn8O16/rGO, self-assembled by Ag1.8Mn8O16 nanorods and reduced graphene oxide (rGO) nanosheets through electrostatic attraction. The hybrid catalyst exhibits a better oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) activity than commercial Pt/C in alkaline medium. When employed as an air-cathode catalyst in Zn-air cells, the hybrids enabled higher and more stable output voltage and better durability of the cells, benefitting from the improved electrode conductivity, larger surface area, and synergetic coupling as a result of its high structural integrity. 相似文献
13.
Xuan Wei Diao Zheng Ming Zhao Dr. Hongzhong Chen Xun Fan Bin Gao Dr. Long Gu Dr. Yi Guo Dr. Jianbin Qin Prof. Jing Wei Prof. Yanli Zhao Prof. Guangcheng Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(34):14747-14754
Heteroatom-doped polymers or carbon nanospheres have attracted broad research interest. However, rational synthesis of these nanospheres with controllable properties is still a great challenge. Herein, we develop a template-free approach to construct cross-linked polyphosphazene nanospheres with tunable hollow structures. As comonomers, hexachlorocyclotriphosphazene provides N and P atoms, tannic acid can coordinate with metal ions, and the replaceable third comonomer can endow the materials with various properties. After carbonization, N/P-doped mesoporous carbon nanospheres were obtained with small particle size (≈50 nm) and high surface area (411.60 m2 g−1). Structural characterization confirmed uniform dispersion of the single atom transition metal sites (i.e., Co-N2P2) with N and P dual coordination. Electrochemical measurements and theoretical simulations revealed the oxygen reduction reaction performance. This work provides a solution for fabricating diverse heteroatom-containing polymer nanospheres and their derived single metal atom doped carbon catalysts. 相似文献
14.
采用溶剂热法合成了以锆为金属核心、2-氨基为配体的锆基金属有机骨架(UiO-66)纳米材料,通过静电纺丝技术制备出UiO-66自由分散的聚丙烯腈(PAN/UiO-66)纤维,可控热解得到多孔碳纳米纤维(porous carbon nanofibers,PCNFs),结合湿化学还原法在PCNFs表面沉积Pd纳米颗粒,得到PCNFs@Pd复合材料。通过扫描电子显微镜、透射电子显微镜、X射线衍射技术对其形貌、组成、结构进行表征;采用电化学工作站分别测试了PCNFs@Pd在0.1 mol·L-1KOH和0.1 mol·L-1HClO4电解质中氧还原性能(oxygen reduction reaction,ORR)。结果表明,在PAN纤维中添加UiO-66显著提高了PCNFs@Pd(Pd负载量为0.34%)复合材料的ORR性能。相比40%Pt/C,在碱性电解质中,PCNFs@Pd复合材料展示出更低的Tafel斜率、更优异的循环稳定性和耐甲醇中毒性。在酸性电解质中也表现出类似20%Pt/C的催化活性和循环稳定性。 相似文献
15.
Dr. Chun-Chao Hou Dr. Lianli Zou Dr. Liming Sun Dr. Kexin Zhang Dr. Zheng Liu Prof. Yinwei Li Dr. Caixia Li Prof. Ruqiang Zou Prof. Jihong Yu Prof. Qiang Xu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(19):7454-7459
Single-atom catalysts have drawn great attention, especially in electrocatalysis. However, most of previous works focus on the enhanced catalytic properties via improving metal loading. Engineering morphologies of catalysts to facilitate mass transport through catalyst layers, thus increasing the utilization of each active site, is regarded as an appealing way for enhanced performance. Herein, we design an overhang-eave structure decorated with isolated single-atom iron sites via a silica-mediated MOF-templated approach for oxygen reduction reaction (ORR) catalysis. This catalyst demonstrates superior ORR performance in both alkaline and acidic electrolytes, comparable to the state-of-the-art Pt/C catalyst and superior to most precious-metal-free catalysts reported to date. This activity originates from its edge-rich structure, having more three-phase boundaries with enhanced mass transport of reactants to accessible single-atom iron sites (increasing the utilization of active sites), which verifies the practicability of such a synthetic approach. 相似文献
16.
金属空气电池阴极氧还原催化剂研究进展 总被引:4,自引:0,他引:4
随着能源危机加剧和生态环境恶化, 可持续发展能源受到更大的重视. 金属空气电池作为一种绿色能源是具有很大发展潜力的新一代电池. 与传统电池相比, 此类电池有着更高的理论能量密度, 尤其是锂空电池, 能量密度可达3505 Wh/kg, 然而阴极缓慢的氧还原反应成为制约其发展的关键因素之一. 在简要介绍氧还原反应机理基础上, 着重介绍了近年来氧还原催化剂如贵金属及其合金、过渡金属氧化物/硫化物、功能化碳材料和金属氮化物的研究进展, 并根据目前所存在问题指出未来研究方向, 包括深入研究氧还原反应机理, 明确催化剂活性位; 研究催化剂结构等对催化活性的影响, 优化制备条件, 以提高催化活性和稳定性; 根据氧还原机理设计开发新型氧还原催化剂. 相似文献
17.
18.
采用D-氨基葡萄糖作为Co分散剂和碳源,硫脲作为氮源和硫源,以NaCl为模板制备负载硫化钴纳米颗粒的N、S共掺杂三维石墨烯氧还原电催化剂(CoS/N/S/rGO)。CoS/N/S/rGO具有良好的氧还原反应(ORR)活性,起始电位和半波电位分别为960和815 mV,性能与商业Pt/C相当。此外,CoS/N/S/rGO表现出明显的4电子转移特性和超低的过氧化氢产率。与基于Pt/C的锌-空气电池相比,基于CoS/N/S/rGO的锌-空气电池在6 mol·L~(-1) KOH和0.2 mol~(-1) Zn(CH_3COO)_2碱性电解质中显示出更高的恒电流放电性能以及更好的稳定性。 相似文献
19.
Xuan Wei Diao Zheng Ming Zhao Hongzhong Chen Xun Fan Bin Gao Long Gu Yi Guo Jianbin Qin Jing Wei Yanli Zhao Guangcheng Zhang 《Angewandte Chemie (International ed. in English)》2020,59(34):14639-14646
Heteroatom‐doped polymers or carbon nanospheres have attracted broad research interest. However, rational synthesis of these nanospheres with controllable properties is still a great challenge. Herein, we develop a template‐free approach to construct cross‐linked polyphosphazene nanospheres with tunable hollow structures. As comonomers, hexachlorocyclotriphosphazene provides N and P atoms, tannic acid can coordinate with metal ions, and the replaceable third comonomer can endow the materials with various properties. After carbonization, N/P‐doped mesoporous carbon nanospheres were obtained with small particle size (≈50 nm) and high surface area (411.60 m2 g?1). Structural characterization confirmed uniform dispersion of the single atom transition metal sites (i.e., Co‐N2P2) with N and P dual coordination. Electrochemical measurements and theoretical simulations revealed the oxygen reduction reaction performance. This work provides a solution for fabricating diverse heteroatom‐containing polymer nanospheres and their derived single metal atom doped carbon catalysts. 相似文献
20.
Dr. Mahendra K. Awasthi Abhishek Saini Chandan Das Anwesha Banerjee Naseer Ahmad Shah Prof. Dr. Goutam Kumar Lahiri Prof. Dr. Arnab Dutta 《欧洲无机化学杂志》2023,26(27):e202300204
The proper utilization of renewable energy sources has emerged as a major challenge in our pursuit of a sustainable and carbon-neutral energy landscape. Small molecule activation is a key component for proper utilization of renewable energy resources, where O2/H2O redox couple is reckoned to be a potential game changer. In this regard, electrocatalytic oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) have become the prime interest of catalyst designers. Typically, these ORR and OER electrocatalysts are developed distinctly; however, very soon, the requirement of a bidirectional ORR/OER electrocatalyst becomes obvious for practical applicability and rapid energy transduction purposes. A bidirectional catalyst is defined as a catalyst capable of driving a redox reaction in opposing directions. This review has portrayed the development of enzyme structure-inspired design of molecular bidirectional ORR/OER catalysts. The strategic incorporation of secondary and outer coordination sphere features has significantly enhanced the performance of these catalysts, which can be monitored via the key catalytic parameters. These bifunctional OER/ORR catalysts are vital for metal-air battery and fuel cell applications and appropriately poised to lay the foundation for an efficient, economical, and eco-friendly pathway for sustainable energy usage with the rational assembly of energy converting and storage devices. 相似文献