The design and preparation of non-noble metal catalysts with high catalytic activity and robust stability are important in the research of metal-air batteries and fuel cells.Here,a three-dimensional(3D)hierarchically ...The design and preparation of non-noble metal catalysts with high catalytic activity and robust stability are important in the research of metal-air batteries and fuel cells.Here,a three-dimensional(3D)hierarchically ordered porous carbon nanomaterial was conveniently synthesized with zeolite-imidazole framework(ZIF-8)carbonization using the silica-template method and carbon nanotube(CNT)growth.The addition of an iron source endows the porous mFeNCCNT with Fe-based nanoparticles and abundant atomically dispersive Fe-Nx sites from its nitrogen-incorporated graphitic carbon matrix.As a result,the 3D porous structure reduces the charge transport resistance,and the iron and nitrogen codoped carbon exhibits excellent catalytic activity for oxygen reduction reaction(ORR)similar to that of commercial Pt/C.Meanwhile,the interwoven CNTs obtained under urea catalysis further shorten the ion and electron diffusion pathway.Experimental and theoretical analyses revealed that the optimized mFeNC-CNT has a high ORR activity with a half-wave potential of 0.908 V and a large open-circuit voltage(1.556 V)when applied on zinc-air batteries.This work provides a promising strategy for the rational design and facile synthesis of high-performing non-noble metal-based electrocatalysts for energy storage,conversion,and transport applications.展开更多
Two novel Co-based clusters with the 2-(hydroxylmethyl)pyridine(hmpH)ligand,formulated as[Co3(hmp)6(hmpH)]×2NO3×3H2O(ZTU-3)and[Co4(hmp)4(CH3CO2)2(H2O)4]×2NO3(ZTU-4),have been successfully synthesized an...Two novel Co-based clusters with the 2-(hydroxylmethyl)pyridine(hmpH)ligand,formulated as[Co3(hmp)6(hmpH)]×2NO3×3H2O(ZTU-3)and[Co4(hmp)4(CH3CO2)2(H2O)4]×2NO3(ZTU-4),have been successfully synthesized and structurally characterized.ZTU-3 features a triangular core geometry,while ZTU-4 exhibits a cuboidal core geometry.In addition,the magnetic properties of ZTU-3 and ZTU-4 are also all investigated.展开更多
基金supported by the National Natural Science Foundation of China (21601137)the Natural Science Foundation of Zhejiang Province (LQ16B010003)the Basic Science and Technology Research Project of Wenzhou, Zhejiang Province (G20190007)。
基金financially supported by the National Natural Science Foundation of China(21601137,51972238,U21A2081,and 22105147)the Basic Science and Technology Research Project of Wenzhou,Zhejiang Province(G20190007)the Special Basic Cooperative Research Programs of Yunnan Provincial Undergraduate Universities Association(202101BA070001-042)。
文摘合理地设计和制备低成本、高效、稳定的非贵金属基碳纳米材料具有重要意义.本文中我们在不同温度条件下,通过有机配体交换将MOF-5转换为ZIF-8,其过程中可以捕捉到ZIF-8的中间态(ZIF-8-M)并得到最终态(ZIF-8-F).将掺杂Fe离子的MOF材料进行热解后,得到的Fe-ZIF-8-F-900材料具有大的比表面积、高的石墨化程度、丰富的碳纳米管以及高活性的铁物种等优点.这些特性有助于后续氧还原反应(ORR)更好的电子转移和质量传输.与Pt/C相比,Fe-ZIF-8-F-900具有优异的ORR性能,如较正的起始电位(0.982 V),大的极限电流密度(5.41 mA cm^(-2))和较小的Tafel斜率(40.6 mV dec^(-1)),且在10小时后电流保持率仍高达94.4%.此外,实验和理论结果均证实了Fe-ZIF-8-F-900组装的锌空气电池在实际应用中表现优异.本研究将为高效、低成本的非贵金属基电催化剂的开发和制备提供合理的设计策略,并为其在能源相关领域的实际应用指明方向.
基金financially supported by the Basic Science and Technology Research Project of Wenzhou,Zhejiang Province(G20190007 and ZG2017027)the BUCT-WZU Joint Fund(KH2012031)the State Key Laboratory of Structural Chemistry,Chinese Academy of Sciences(20190008)。
文摘The design and preparation of non-noble metal catalysts with high catalytic activity and robust stability are important in the research of metal-air batteries and fuel cells.Here,a three-dimensional(3D)hierarchically ordered porous carbon nanomaterial was conveniently synthesized with zeolite-imidazole framework(ZIF-8)carbonization using the silica-template method and carbon nanotube(CNT)growth.The addition of an iron source endows the porous mFeNCCNT with Fe-based nanoparticles and abundant atomically dispersive Fe-Nx sites from its nitrogen-incorporated graphitic carbon matrix.As a result,the 3D porous structure reduces the charge transport resistance,and the iron and nitrogen codoped carbon exhibits excellent catalytic activity for oxygen reduction reaction(ORR)similar to that of commercial Pt/C.Meanwhile,the interwoven CNTs obtained under urea catalysis further shorten the ion and electron diffusion pathway.Experimental and theoretical analyses revealed that the optimized mFeNC-CNT has a high ORR activity with a half-wave potential of 0.908 V and a large open-circuit voltage(1.556 V)when applied on zinc-air batteries.This work provides a promising strategy for the rational design and facile synthesis of high-performing non-noble metal-based electrocatalysts for energy storage,conversion,and transport applications.
基金Supported by the National Natural Science Foundation of China(21861044 and 21601137)the Project funded by China Postdoctoral Science Foundation(2018M633426)the Project funded by Yunnan Province Postdoctoral Science Foundation
文摘Two novel Co-based clusters with the 2-(hydroxylmethyl)pyridine(hmpH)ligand,formulated as[Co3(hmp)6(hmpH)]×2NO3×3H2O(ZTU-3)and[Co4(hmp)4(CH3CO2)2(H2O)4]×2NO3(ZTU-4),have been successfully synthesized and structurally characterized.ZTU-3 features a triangular core geometry,while ZTU-4 exhibits a cuboidal core geometry.In addition,the magnetic properties of ZTU-3 and ZTU-4 are also all investigated.
