超级交换
钙钛矿(结构)
催化作用
盐(化学)
选择性
八面体
氧化物
金属
无机化学
电子转移
化学
材料科学
离子
晶体结构
结晶学
物理化学
生物化学
有机化学
作者
Jiawei Zhu,Yu Zhang,Zitao Chen,Zhenbao Zhang,Xuezeng Tian,Minghua Huang,Xuedong Bai,Xue Wang,Yongfa Zhu,Heqing Jiang
标识
DOI:10.1038/s41467-024-45747-5
摘要
Abstract Cu-oxide-based catalysts are promising for CO 2 electroreduction (CO 2 RR) to CH 4 , but suffer from inevitable reduction (to metallic Cu) and uncontrollable structural collapse. Here we report Cu-based rock-salt-ordered double perovskite oxides with superexchange-stabilized long-distance Cu sites for efficient and stable CO 2 -to-CH 4 conversion. For the proof-of-concept catalyst of Sr 2 CuWO 6 , its corner-linked CuO 6 and WO 6 octahedral motifs alternate in all three crystallographic dimensions, creating sufficiently long Cu-Cu distances (at least 5.4 Å) and introducing marked superexchange interaction mainly manifested by O-anion-mediated electron transfer (from Cu to W sites). In CO 2 RR, the Sr 2 CuWO 6 exhibits significant improvements (up to 14.1 folds) in activity and selectivity for CH 4 , together with well boosted stability, relative to a physical-mixture counterpart of CuO/WO 3 . Moreover, the Sr 2 CuWO 6 is the most effective Cu-based-perovskite catalyst for CO 2 methanation, achieving a remarkable selectivity of 73.1% at 400 mA cm −2 for CH 4 . Our experiments and theoretical calculations highlight the long Cu-Cu distances promoting *CO hydrogenation and the superexchange interaction stabilizing Cu sites as responsible for the superb performance.
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