Gas Diffusion Strategy for Inserting Atomic Iron Sites into Graphitized Carbon Supports for Unusually High-Efficient CO2 Electroreduction and High-Performance Zn-CO2 Batteries
Gas Diffusion Strategy for Inserting Atomic Iron Sites into Graphitized Carbon Supports for Unusually High-Efficient CO2 Electroreduction and High-Performance Zn-CO2 Batteries
复制标题
将原子铁位点插入石墨化碳载体中的气体扩散策略，用于异常高效的 CO2 电还原和高性能 Zn-CO2 电池
DOI：
10.1002/adma.202002430
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发表时间：
2020
影响因子：
29.4
通讯作者：
Hou Yang
中科院分区：
文献类型：
--
作者：
Wang Tingting;Sang Xiahan;Zheng Wanzhen;Yang Bin;Yao Siyu;Lei Chaojun;Li Zhongjian;He Qinggang;Lu Jianguo;Lei Lecheng;Dai Liming;Hou Yang
新兴的单原子催化剂（SACs）在二氧化碳电还原（CO2ER）方面具有很大的前景，但设计高活性和低成本的SACs仍然具有挑战性。本文提出了一种气体扩散策略，以及一步热活化，用于制造含有微量分离铁原子的N掺杂多孔碳多面体（Fe1NC）。优化后的Fe1NC/S1‐1000具有N掺杂石墨碳负载的Fe‐n3原子位，具有优异的CO2ER性能，在- 0.5 V下CO法拉第效率高达96%，周转率为2225 h−1，并且具有出色的稳定性，优于几乎所有基于N掺杂碳负载的非贵金属的sac。所观察到的优异的CO2ER性能是由于通过尺寸调制和热活化的再分配增加的电化学表面积大大提高了活性中心的可及性和固有活性。实验观察和理论计算表明，Fe‐n3位点对*COOH和*CO中间体具有平衡的吸附能，有利于CO的形成。通用气体扩散策略用于生产一系列具有单铁原子的尺寸控制碳负载SACs，同时开发了以Fe1NC/S1‐1000为阴极的可充电zn - co2电池，其最大功率密度为0.6 mW cm - 2。
Emerging single‐atom catalysts (SACs) hold great promise for CO2electroreduction (CO2ER),but the design of highly active and cost‐efficient SACs is still challenging. Herein, a gas diffusion strategy, along with one‐step thermal activation, for fabricating N‐doped porous carbon polyhedrons with trace isolated Fe atoms (Fe1NC) is developed. The optimized Fe1NC/S1‐1000 with atomic Fe‐N3sites supported by N‐doped graphitic carbons exhibits superior CO2ER performance with the CO Faradaic efficiency up to 96% at −0.5 V, turnover frequency of 2225 h−1, and outstanding stability, outperforming almost all previously reported SACs based on N‐doped carbon supported nonprecious metals. The observed excellent CO2ER performance is attributed to the greatly enhanced accessibility and intrinsic activity of active centers due to the increased electrochemical surface area through size modulation and the redistribution of doped N species by thermal activation. Experimental observations and theoretical calculations reveal that the Fe‐N3sites possess balanced adsorption energies of *COOH and *CO intermediates, facilitating CO formation. A universal gas diffusion strategy is used to exclusively yield a series of dimension‐controlled carbon‐supported SACs with single Fe atoms while a rechargeable Zn–CO2battery with Fe1NC/S1‐1000 as cathode is developed to deliver a maximal power density of 0.6 mW cm−2.