电催化剂
材料科学
多孔性
蜂巢
异质结
吸附
金属有机骨架
化学工程
密度泛函理论
纳米技术
物理化学
电化学
电极
复合材料
计算化学
化学
光电子学
工程类
作者
Yi‐Lu Yang,Yi‐Rong Wang,Long‐Zhang Dong,Qi Li,Lei Zhang,Jie Zhou,Shengnan Sun,Huimin Ding,Yifa Chen,Shunli Li,Ya‐Qian Lan
标识
DOI:10.1002/adma.202206706
摘要
Porous heterostructured electrocatalysts with multifunctionality and synergistic effect have much benefit for efficient electrocatalytic CO2 reduction reaction (CO2 RR), yet it still remains a daunting challenge to explore heterostructures based on covalent organic frameworks (COFs) and metal-organic frameworks (MOFs) in this field. Here, a series of honeycomb-like porous crystalline hetero-electrocatalysts (MCH-X, X = 1-4, X stands for the numbered sample obtained from different MOF doses in the synthesis of the MCH) are synthesized, and these are successfully applied in electrocatalytic CO2 RR. The specially designed heterostructures with integrated porous MOF-template and ultrathin COF-coating enable efficient CO2 adsorption/activation and conversion into CH4 . The best of them, MCH-3, shows greatly inhibited H2 evolution, excellent current density (-398.1 mA cm-2 ), and superior FECH4${\rm{F}}{{\rm{E}}_{{\rm{C}}{{\rm{H}}_4}}}$ (76.7%) to the physical mixture (38.0%), the MOF@COF without the honeycomb-like morphology (47.7%), and the bare COF (37.5%) and MOF (15.9%) at -1.0 V. Based on the density functional theory calculations and various characterizations, the vital roles of the MOF in facilitating CO2 adsorption/activation, stabilizing intermediates, and conquering the energy barrier of rate-determining step are intensively studied.
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