Cation-Deficiency-Dependent CO2 Electroreduction over Copper-Based Ruddlesden-Popper Perovskite Oxides.
Cation-Deficiency-Dependent CO2 Electroreduction over Copper-Based Ruddlesden-Popper Perovskite Oxides.
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DOI：
10.1002/anie.202111670
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发表时间：
2021-10
影响因子：
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通讯作者：
Jiawei Zhu;Yanying Wang;Aomiao Zhi;Zitao Chen;Lei Shi;Zhenbao Zhang;Yu Zhang;Yinlong Zhu;X. Qiu;Xuezeng Tian;X. Bai;Ying Zhang;Yong Zhu
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文献类型：
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作者：
Jiawei Zhu;Yanying Wang;Aomiao Zhi;Zitao Chen;Lei Shi;Zhenbao Zhang;Yu Zhang;Yinlong Zhu;X. Qiu;Xuezeng Tian;X. Bai;Ying Zhang;Yong Zhu
Here we report an effective strategy to enhance CO2 electroreduction (CER) properties of Cu-based Ruddlesden-Popper (RP) perovskite oxides by engineering their A-site cation deficiencies. With La2-xCuO4-δ (L2-xC, x = 0, 0.1, 0.2, and 0.3) as proof-of-concept catalysts, we demonstrate that their CER activity and selectivity (to C2+ or CH4) show either a volcano-type or an inverted volcano-type dependence on the x values, with the extreme point at x = 0.1. Among them, at -1.4 V, the L1.9C delivers the optimal activity (51.3 mA·cm-2) and selectivity (41.5%) for C2+, comparable to or better than those of most reported Cu-based oxides, while the L1.7C exhibits the best activity (25.1 mA·cm-2) and selectivity (22.1%) for CH4. Such optimized CER properties could be ascribed to the favorable merits brought by the cation-deficiency-induced oxygen vacancies and/or CuO/RP hybrids, including the facilitated adsorption/activation of key reaction species and thus the manipulated reaction pathways.
