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Tuning the atomic configuration environment of MnN_(4) sites by Co cooperation for efficient oxygen reduction

Journal of Energy Chemistry 2023年第7期82卷 547-559,I0012页

作者： Jing Wang Haihong Zhong Jun Yang Huiyu Li Pinggui Tang Yongjun Feng Dianqing Li State Key Laboratory of Chemical Resource Engineering Beijing Engineering Center for Hierarchical CatalystsCollege of ChemistryBeijing University of Chemical TechnologyBeijing 100029China College of Science Hainan UniversityHaikou 570228HainanChina State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

Carbon-based N-coordinated Mn(Mn-N_(x)/C)single-atom electrocatalysts are considered as one of the most desirable non-precious oxygen reduction reaction(ORR)candidates due to their insignificant Fenton reactivity,high abundance,and intriguing electrocatalytic performance.However,current MnN_(x)/C single-atom electrocatalysts suffer from high overpotentials because of their low intrinsic activity and unsatisfactory chemical stability.Herein,through an in-situ polymerization-assisted pyrolysis,the Co as a second metal is introduced into the Mn-N_(x)/C system to construct Co,Mn-N_(x)dual-metallic sites,which atomically disperse in N-doped 1D carbon nanorods,denoted as Co,Mn-N/CNR and hereafter.Using electron microscopy and X-ray absorption spectroscopy(XAS)techniques,we verify the uniform dispersion of CoN4and MnN4atomic sites and confirm the effect of Co doping on the MnN_(4) electronic structure.Density functional theory(DFT)calculations further elucidate that the energy barrier of ratedetermining step(^(*)OH desorption)decreases over the 2 N-bridged MnCoN_(6) moieties related to the pure MnN_(4).This work provides an effective strategy to modulate the local coordination environment and electronic structure of MnN_(4) active sites for improving their ORR activity and stability.

关键词： dual-atom sites Oxygen reduction reaction M-Nx/C catalysts Coordination environment Electronic structure Synergistic effect

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Engineering Electronic Density and Coordination Environment of Mn–Nx sites via Zn Cooperation for Quasi-Solid-State Zinc-Air Batteries

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Renewables 2023年第3期1卷 362-372页

作者： Daijie Deng Huixin Ma Suqin Wu Huan Wang Junchao Qian Jianchun Wu Huaming Li Cheng Yan Henan Li Li Xu Institute for Energy Research School of Chemistry and Chemical EngineeringSchool of Materials Science and EngineeringJiangsu UniversityZhenjiang 212013Jiangsu Jiangsu Key Laboratory for Environment Functional Materials Suzhou University of Science and TechnologySuzhou 215009Jiangsu Key Laboratory of Radio Frequency and Micro-Nano Electronics of Jiangsu Province Nanjing 210023 School of Mechanical Medical and Process EngineeringQueensland University of TechnologyBrisbaneQueensland 4001

Due to the poor Fenton reactivity,single-atom Mn-based materials are generally identified as one of the most promising active catalysts for oxygen reduction reaction(ORR).Regulating the electronic density and coordination environment of atomically dispersed Mn centers is an effective strategy to enhance ORR activity of Mn-based materials.By introducing Zn sites,atomically dispersed Mn centers with multitudes of coordination(including Zn/Mn–Nx and Mn–Nx moieties)can be constructed to form Mn-based ORR catalyst(Zn/Mn-NC)with dual-atom sites.Around Mn–Nx sites,the Zn atoms can effectively modulate the electronic structure and coordination state of Mn centers in Zn/Mn-NC through d–d orbital coupling.The electronic interaction between Zn and Mn sites improves ORR activity,thereby optimizing the oxygen adsorption energy of Mn sites in Zn/Mn-NC and reducing the overall energy barrier.Zn/Mn-NC displays higher ORR half-wave potential than Pt/C(0.89 V vs 0.86 V).The quasi-solid-state zinc-air battery(ZAB)with Zn/Mn-NC as the cathode displayed excellent rechargeability,recyclability,and mechanical robustness.The strategy presented regulates the electronic density and coordination environment of singleatom Mn-based ORR catalysts in quasi-solid-state ZABs.

关键词： quasi-solid-state zinc-air batteries oxygen reduction reaction dual-atom sites Mn-Nx Zn/Mn-Nx

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