Bimetal–Organic Framework Self-Adjusted Synthesis of Support-Free Nonprecious Electrocatalysts for Efficient Oxygen Reduction

You, Bo; Jiang, Nan; Sheng, Meili; Drisdell, Walter S.; Yano, Junko; Sun, Yujie

doi:10.1021/acscatal.5b02325

Bimetal–Organic Framework Self-Adjusted Synthesis of Support-Free Nonprecious Electrocatalysts for Efficient Oxygen Reduction

Journal Article · Thu Oct 22 00:00:00 EDT 2015 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.5b02325· OSTI ID:1397236

You, Bo ^[1]; Jiang, Nan ^[1]; Sheng, Meili ^[1]; Drisdell, Walter S. ^[2]; Yano, Junko ^[3]; Sun, Yujie ^[1]

Utah State Univ., Logan, UT (United States)
Joint Center of Artificial Photosynthesis, Berkeley, CA (United States)
Joint Center of Artificial Photosynthesis, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

The development of low-cost catalysts with oxygen reduction reaction (ORR) activity superior to that of Pt for fuel cells is highly desirable but remains challenging. Herein, we report a bimetal-organic framework (bi-MOF) self-adjusted synthesis of support-free porous Co-N-C nanopolyhedron electrocatalysts by pyrolysis of a Zn/Co bi-MOF without any post-treatments. The presence of initial Zn forms a spatial isolation of Co that suppresses its sintering during pyrolysis, and Zn evaporation also promotes the surface area of the resultant catalysts. The composition, morphology, and hence ORR activity of Co-N-C could be tuned by the Zn/Co ratio. The optimal Co-N-C exhibited remarkable ORR activity with a half-wave potential of 0.871 V versus the reversible hydrogen electrode (RHE) (30 mV more positive than that of commercial 20 wt % Pt/C) and a kinetic current density of 39.3 mA cm^-2 at 0.80 V versus RHE (3.1 times that of Pt/C) in 0.1 M KOH, and excellent stability and methanol tolerance. It also demonstrated ORR activity comparable to and stability much higher than those of Pt/C in acidic and neutral electrolytes. Various characterization techniques, including X-ray absorption spectroscopy, revealed that the superior activity and strong stability of Co-N-C originated from the intense interaction between Co and N, the high content of ORR active pyridinic and pyrrolic N, and the large specific surface area.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1397236

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 12 Vol. 5; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Microporous Solids En Route to Heterogeneous Electrocatalysis: The Oxygen Reduction Reaction Haikal, Rana R.; Hassan, Mohamed H.; Alkordi, Mohamed H. Energy Technology, Vol. 8, Issue 3 https://doi.org/10.1002/ente.201900964	journal	December 2019
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Self-Templated Synthesis of Co- and N-Doped Carbon Microtubes Composed of Hollow Nanospheres and Nanotubes for Efficient Oxygen Reduction Reaction Ahn, Sung Hoon; Manthiram, Arumugam Small, Vol. 13, Issue 11 https://doi.org/10.1002/smll.201603437	journal	January 2017
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Porous Carbon-Hosted Atomically Dispersed Iron-Nitrogen Moiety as Enhanced Electrocatalysts for Oxygen Reduction Reaction in a Wide Range of pH Fu, Shaofang; Zhu, Chengzhou; Su, Dong Small, Vol. 14, Issue 12 https://doi.org/10.1002/smll.201703118	journal	February 2018
Sustainable Synthesis of Co@NC Core Shell Nanostructures from Metal Organic Frameworks via Mechanochemical Coordination Self-Assembly: An Efficient Electrocatalyst for Oxygen Reduction Reaction Peera, Shaik Gouse; Balamurugan, Jayaraman; Kim, Nam Hoon Small, Vol. 14, Issue 19 https://doi.org/10.1002/smll.201800441	journal	April 2018
UIO-66-NH ₂ -Derived Mesoporous Carbon Catalyst Co-Doped with Fe/N/S as Highly Efficient Cathode Catalyst for PEMFCs Zheng, Long; Dong, Yuanyuan; Chi, Bin Small, Vol. 15, Issue 4 https://doi.org/10.1002/smll.201803520	journal	December 2018
Pyridinic‐N Protected Synthesis of 3D Nitrogen‐Doped Porous Carbon with Increased Mesoporous Defects for Oxygen Reduction Luo, Jin; Wang, Kangjun; Hua, Xing Small, Vol. 15, Issue 11 https://doi.org/10.1002/smll.201805325	journal	February 2019
Enhanced Electrocatalytic Performance through Body Enrichment of Co‐Based Bimetallic Nanoparticles In Situ Embedded Porous N‐Doped Carbon Spheres Song, Qianqian; Li, Junqi; Wang, Shaolan Small, Vol. 15, Issue 44 https://doi.org/10.1002/smll.201903395	journal	September 2019
Cobalt@Nitrogen‐Doped Porous Carbon Fiber Derived from the Electrospun Fiber of Bimetal–Organic Framework for Highly Active Oxygen Reduction Bai, Qing; Shen, Feng‐Cui; Li, Shun‐Li Small Methods, Vol. 2, Issue 12 https://doi.org/10.1002/smtd.201800049	journal	May 2018
NiS‐Decorated ZnO/ZnS Nanorod Heterostructures for Enhanced Photocatalytic Hydrogen Production: Insight into the Role of NiS Zhang, Qingsong; Xiao, Yang; Li, Yiming Solar RRL, Vol. 4, Issue 4 https://doi.org/10.1002/solr.201900568	journal	April 2020
Metal–Organic Frameworks for Electrocatalysis Usman, Muhammad; Zhu, Qi-Long Methods for Electrocatalysis: Advanced Materials and Allied Applications, p. 29-66 https://doi.org/10.1007/978-3-030-27161-9_2	book	January 2020
Facile in situ fabrication of Co nanoparticles embedded in 3D N-enriched mesoporous carbon foam electrocatalyst with enhanced activity and stability toward oxygen reduction reaction Xu, Chunyang; Lin, Zheng; Zhao, Dian Journal of Materials Science, Vol. 54, Issue 7 https://doi.org/10.1007/s10853-018-03255-0	journal	January 2019
Strategies for Enhancing the Electrocatalytic Activity of M–N/C Catalysts for the Oxygen Reduction Reaction Sa, Young Jin; Woo, Jinwoo; Joo, Sang Hoon Topics in Catalysis, Vol. 61, Issue 9-11 https://doi.org/10.1007/s11244-018-0935-0	journal	May 2018
Metal-organic framework based nanomaterials for electrocatalytic oxygen redox reaction Zhang, Kexin; Guo, Wenhan; Liang, Zibin Science China Chemistry, Vol. 62, Issue 4 https://doi.org/10.1007/s11426-018-9441-4	journal	March 2019
Metal-organic framework-derived, Zn-doped porous carbon polyhedra with enhanced activity as bifunctional catalysts for rechargeable zinc-air batteries Wu, Xuan; Meng, Ge; Liu, Wenxian Nano Research, Vol. 11, Issue 1 https://doi.org/10.1007/s12274-017-1615-2	journal	July 2017
Conversion of confined metal@ZIF-8 structures to intermetallic nanoparticles supported on nitrogen-doped carbon for electrocatalysis Qi, Zhiyuan; Pei, Yuchen; Goh, Tian Wei Nano Research, Vol. 11, Issue 6 https://doi.org/10.1007/s12274-018-2016-x	journal	May 2018
Metal–Organic Frameworks (MOFs) and MOF-Derived Materials for Energy Storage and Conversion Zhang, Xu; Chen, An; Zhong, Ming Electrochemical Energy Reviews, Vol. 2, Issue 1 https://doi.org/10.1007/s41918-018-0024-x	journal	November 2018
Metal-Nitrogen-Carbon Catalysts for Oxygen Reduction in PEM Fuel Cells: Self-Template Synthesis Approach to Enhancing Catalytic Activity and Stability He, Yanghua; Tan, Qiang; Lu, Leilei Electrochemical Energy Reviews, Vol. 2, Issue 2 https://doi.org/10.1007/s41918-019-00031-9	journal	March 2019
Achievements, challenges and perspectives on cathode catalysts in proton exchange membrane fuel cells for transportation Wang, Xiao Xia; Swihart, Mark T.; Wu, Gang Nature Catalysis, Vol. 2, Issue 7 https://doi.org/10.1038/s41929-019-0304-9	journal	July 2019
Switching effective oxygen reduction and evolution performance by controlled graphitization of a cobalt–nitrogen–carbon framework system Gadipelli, Srinivas; Zhao, Tingting; Shevlin, Stephen A. Energy & Environmental Science, Vol. 9, Issue 5 https://doi.org/10.1039/c6ee00551a	journal	January 2016
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Unusual formation of tetragonal microstructures from nitrogen-doped carbon nanocapsules with cobalt nanocores as a bi-functional oxygen electrocatalyst Hu, Enlai; Ning, Jiqiang; He, Bin Journal of Materials Chemistry A, Vol. 5, Issue 5 https://doi.org/10.1039/c6ta09943b	journal	January 2017
Recent advances in air electrodes for Zn–air batteries: electrocatalysis and structural design Cai, Xiaoyi; Lai, Linfei; Lin, Jianyi Materials Horizons, Vol. 4, Issue 6 https://doi.org/10.1039/c7mh00358g	journal	January 2017
Metal organic frameworks as precursors for the manufacture of advanced catalytic materials Oar-Arteta, Lide; Wezendonk, Tim; Sun, Xiaohui Materials Chemistry Frontiers, Vol. 1, Issue 9 https://doi.org/10.1039/c7qm00007c	journal	January 2017
Bimetallic zeolitic imidazolate frameworks-derived porous carbon-based materials with efficient synergistic microwave absorption properties: the role of calcining temperature Wang, Suyun; Ke, Xiang; Zhong, Suting RSC Adv., Vol. 7, Issue 73 https://doi.org/10.1039/c7ra08882e	journal	January 2017
Synthesis of CrO _x /C catalysts for low temperature NH ₃ -SCR with enhanced regeneration ability in the presence of SO ₂ Yu, Shuohan; Xu, Sheng; Sun, Bowen RSC Advances, Vol. 8, Issue 7 https://doi.org/10.1039/c7ra09680a	journal	January 2018
Graphene oxide/core–shell structured metal–organic framework nano-sandwiches and their derived cobalt/N-doped carbon nanosheets for oxygen reduction reactions Wei, Jing; Hu, Yaoxin; Liang, Yan Journal of Materials Chemistry A, Vol. 5, Issue 21 https://doi.org/10.1039/c7ta00276a	journal	January 2017
In situ directional formation of Co@CoO _x -embedded 1D carbon nanotubes as an efficient oxygen electrocatalyst for ultra-high rate Zn–air batteries Lin, Chao; Shinde, Sambhaji S.; Jiang, Zheng Journal of Materials Chemistry A, Vol. 5, Issue 27 https://doi.org/10.1039/c7ta02215h	journal	January 2017
Creation of oxygen reduction reaction active sites on titanium oxynitride without increasing the nitrogen doping level Chisaka, Mitsuharu Physical Chemistry Chemical Physics, Vol. 20, Issue 23 https://doi.org/10.1039/c8cp01420e	journal	January 2018
Hierarchically porous Fe–N–C nanospindles derived from a porphyrinic coordination network for oxygen reduction reaction Hua, Xing; Luo, Jin; Shen, Chencheng Catalysis Science & Technology, Vol. 8, Issue 7 https://doi.org/10.1039/c8cy00168e	journal	January 2018
Highly active atomically dispersed CoN ₄ fuel cell cathode catalysts derived from surfactant-assisted MOFs: carbon-shell confinement strategy He, Yanghua; Hwang, Sooyeon; Cullen, David A. Energy & Environmental Science, Vol. 12, Issue 1 https://doi.org/10.1039/c8ee02694g	journal	January 2019
Multi-heteroatom doped graphene-like carbon nanospheres with 3D inverse opal structure: a promising bisphenol-A remediation material Wang, Weixue; Wang, Xiangxue; Xing, Jinlu Environmental Science: Nano, Vol. 6, Issue 3 https://doi.org/10.1039/c8en01196f	journal	January 2019
Enhanced heterogeneous activation of peroxymonosulfate by Co and N codoped porous carbon for degradation of organic pollutants: the synergism between Co and N Wang, Guanlong; Nie, Xiaowa; Ji, Xiaojing Environmental Science: Nano, Vol. 6, Issue 2 https://doi.org/10.1039/c8en01231h	journal	January 2019
Highly-efficient and magnetically-separable ZnO/Co@N-CNTs catalyst for hydrodeoxygenation of lignin and its derived species under mild conditions Ranaware, Virendra; Verma, Deepak; Insyani, Rizki Green Chemistry, Vol. 21, Issue 5 https://doi.org/10.1039/c8gc03623c	journal	January 2019
Mesoporous-silica induced doped carbon nanotube growth from metal–organic frameworks Zhou, Huang; He, Daping; Saana, Amiinu Ibrahim Nanoscale, Vol. 10, Issue 13 https://doi.org/10.1039/c8nr00137e	journal	January 2018
Uniquely integrated Fe-doped Ni(OH) ₂ nanosheets for highly efficient oxygen and hydrogen evolution reactions Ren, Jin-Tao; Yuan, Ge-Ge; Weng, Chen-Chen Nanoscale, Vol. 10, Issue 22 https://doi.org/10.1039/c8nr01655k	journal	January 2018
Reactive template-induced core–shell FeCo@C microspheres as multifunctional electrocatalysts for rechargeable zinc–air batteries Xu, Yanting; Chen, Binling; Nie, Jun Nanoscale, Vol. 10, Issue 36 https://doi.org/10.1039/c8nr02492h	journal	January 2018
Well-dispersed Ni or MnO nanoparticles on mesoporous carbons: preparation via carbonization of bimetallic MOF-74s for highly reactive redox catalysts Bhadra, Biswa Nath; Jhung, Sung Hwa Nanoscale, Vol. 10, Issue 31 https://doi.org/10.1039/c8nr04262d	journal	January 2018
MOF derived carbon based nanocomposite materials as efficient electrocatalysts for oxygen reduction and oxygen and hydrogen evolution reactions Bhattacharyya, Sohini; Das, Chayanika; Maji, Tapas Kumar RSC Advances, Vol. 8, Issue 47 https://doi.org/10.1039/c8ra05102j	journal	January 2018
From a ZIF-8 polyhedron to three-dimensional nitrogen doped hierarchical porous carbon: an efficient electrocatalyst for the oxygen reduction reaction Xuan, Cuijuan; Hou, Baoshan; Xia, Weiwei Journal of Materials Chemistry A, Vol. 6, Issue 23 https://doi.org/10.1039/c8ta02385a	journal	January 2018
In situ derived Fe/N/S-codoped carbon nanotubes from ZIF-8 crystals as efficient electrocatalysts for the oxygen reduction reaction and zinc–air batteries Jin, Huihui; Zhou, Huang; Li, Wenqiang Journal of Materials Chemistry A, Vol. 6, Issue 41 https://doi.org/10.1039/c8ta07849a	journal	January 2018
Integrating MXene nanosheets with cobalt-tipped carbon nanotubes for an efficient oxygen reduction reaction Chen, Jianian; Yuan, Xiaolei; Lyu, Fenglei Journal of Materials Chemistry A, Vol. 7, Issue 3 https://doi.org/10.1039/c8ta10574j	journal	January 2019
A novel Mn/Co dual nanoparticle decorated hierarchical carbon structure derived from a biopolymer hydrogel as a highly efficient electro-catalyst for the oxygen reduction reaction Cao, Lujie; Wang, Zhenyu; Liu, Jinlong Chemical Communications, Vol. 55, Issue 92 https://doi.org/10.1039/c9cc07751k	journal	January 2019
Highly dispersed Co nanoparticles decorated on a N-doped defective carbon nano-framework for a hybrid Na–air battery Zhu, Jingyi; Qu, Tao; Su, Fengmei Dalton Transactions, Vol. 49, Issue 6 https://doi.org/10.1039/c9dt04073k	journal	January 2020
High-performance fuel cell cathodes exclusively containing atomically dispersed iron active sites Zhang, Hanguang; Chung, Hoon T.; Cullen, David A. Energy & Environmental Science, Vol. 12, Issue 8 https://doi.org/10.1039/c9ee00877b	journal	January 2019
Multiscale porous Fe–N–C networks as highly efficient catalysts for the oxygen reduction reaction Li, Ying; Liu, Tong; Yang, Wenxiu Nanoscale, Vol. 11, Issue 41 https://doi.org/10.1039/c9nr05726a	journal	January 2019
Carbon quantum dots enhanced the activity for the hydrogen evolution reaction in ruthenium-based electrocatalysts Li, Weidong; Wei, Zhihong; Wang, Boyang Materials Chemistry Frontiers, Vol. 4, Issue 1 https://doi.org/10.1039/c9qm00618d	journal	January 2020
Tunable and convenient synthesis of highly dispersed Fe–N _x catalysts from graphene-supported Zn–Fe-ZIF for efficient oxygen reduction in acidic media Yang, Limeng; Shao, Zhigang RSC Advances, Vol. 9, Issue 72 https://doi.org/10.1039/c9ra08867a	journal	January 2019
Harnessing MOF materials in photovoltaic devices: recent advances, challenges, and perspectives Chueh, Chu-Chen; Chen, Chih-I; Su, Yu-An Journal of Materials Chemistry A, Vol. 7, Issue 29 https://doi.org/10.1039/c9ta03595h	journal	January 2019
A KCl-assisted pyrolysis strategy to fabricate nitrogen-doped carbon nanotube hollow polyhedra for efficient bifunctional oxygen electrocatalysts Liang, Qiannan; Chen, Zhijie; Chen, Xiaodong Journal of Materials Chemistry A, Vol. 7, Issue 35 https://doi.org/10.1039/c9ta07481c	journal	January 2019
Cobalt/zinc dual-sites coordinated with nitrogen in nanofibers enabling efficient and durable oxygen reduction reaction in acidic fuel cells Zang, Jian; Wang, Feiteng; Cheng, Qingqing Journal of Materials Chemistry A, Vol. 8, Issue 7 https://doi.org/10.1039/c9ta12207a	journal	January 2020
From IR to x-rays: gaining molecular level insights on metal-organic frameworks through spectroscopy Hanna, Lauren; Lockard, Jenny V. Journal of Physics: Condensed Matter, Vol. 31, Issue 48 https://doi.org/10.1088/1361-648x/ab38da	journal	August 2019
In situ -generated NiCo@NiS nanoparticle anchored s-doped carbon nanotubes as dual electrocatalysts for oxygen reduction reaction and hydrogen evolution reaction Ding, Qianqian; Cheng, Aozhi; Ma, Liang Nanotechnology, Vol. 31, Issue 13 https://doi.org/10.1088/1361-6528/ab6007	journal	January 2020
Effective Oxygen Reduction and Evolution Catalysts Derived from Metal Organic Frameworks by Optimizing Active Sites Li, Yanqiang; Xu, Haibin; Huang, Huiyong Journal of The Electrochemical Society, Vol. 165, Issue 3 https://doi.org/10.1149/2.0771803jes	journal	January 2018
Transition Metal–Nitrogen–Carbon (M–N–C) Catalysts for Oxygen Reduction Reaction. Insights on Synthesis and Performance in Polymer Electrolyte Fuel Cells Osmieri, Luigi ChemEngineering, Vol. 3, Issue 1 https://doi.org/10.3390/chemengineering3010016	journal	February 2019
Metal–Organic Frameworks and Their Derivatives for Photocatalytic Water Splitting Song, Fuzhan; Li, Wei; Sun, Yujie Inorganics, Vol. 5, Issue 3, p. 40 https://doi.org/10.3390/inorganics5030040	journal	June 2017

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