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Promoting CO2 Electroreduction Over Nano-Socketed Cu/Perovskite Heterostructures via A-Site-Valence-Controlled Oxygen Vacancies
Small ( IF 13.0 ) Pub Date : 2024-03-13 , DOI: 10.1002/smll.202400615
Mingfa Chen 1 , Yunze Xu 2, 3 , Yu Zhang 2, 3 , Zhenbao Zhang 4 , Xueyan Li 2, 5 , Qi Wang 2, 3 , Minghua Huang 5 , Wei Fang 6 , Yu Zhang 7 , Heqing Jiang 2, 3 , Yongfa Zhu 8 , Jiawei Zhu 1, 2, 3
Small ( IF 13.0 ) Pub Date : 2024-03-13 , DOI: 10.1002/smll.202400615
Mingfa Chen 1 , Yunze Xu 2, 3 , Yu Zhang 2, 3 , Zhenbao Zhang 4 , Xueyan Li 2, 5 , Qi Wang 2, 3 , Minghua Huang 5 , Wei Fang 6 , Yu Zhang 7 , Heqing Jiang 2, 3 , Yongfa Zhu 8 , Jiawei Zhu 1, 2, 3
Affiliation
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Despite the intriguing potential, nano-socketed Cu/perovskite heterostructures for CO2 electroreduction (CO2RR) are still in their infancy and rational optimization of their CO2RR properties is lacking. Here, an effective strategy is reported to promote CO2-to-C2+ conversion over nano-socketed Cu/perovskite heterostructures by A-site-valence-controlled oxygen vacancies. For the proof-of-concept catalysts of Cu/La0.3-xSr0.6+xTiO3-δ (x from 0 to 0.3), their oxygen vacancy concentrations increase controllably with the decreased A-site valences (or the increased x values). In flow cells, their activity and selectivity for C2+ present positive correlations with the oxygen vacancy concentrations. Among them, the Cu/Sr0.9TiO3-δ with most oxygen vacancies shows the optimal activity and selectivity for C2+. And relative to the Cu/La0.3Sr0.6TiO3-δ with minimum oxygen vacancies, the Cu/Sr0.9TiO3-δ exhibits marked improvements (up to 2.4 folds) in activity and selectivity for C2+. The experiments and theoretical calculations suggest that the optimized performance can be attributed to the merits provided by oxygen vacancies, including the accelerated charge transfer, enhanced adsorption/activation of reaction species, and reduced energy barrier for C─C coupling. Moreover, when explored in a membrane-electrode assembly electrolyzer, the Cu/Sr0.9TiO3-δ catalyst shows excellent activity, selectivity (43.9%), and stability for C2H4 at industrial current densities, being the most effective perovskite-based catalyst for CO2-to-C2H4 conversion.
中文翻译：
通过 A 位价控制的氧空位促进纳米插座铜/钙钛矿异质结构上的 CO2 电还原
尽管具有令人着迷的潜力，但用于CO 2电还原（CO 2 RR）的纳米套接字Cu/钙钛矿异质结构仍处于起步阶段，并且缺乏对其CO 2 RR性能的合理优化。在此，报道了一种有效的策略，通过A位价控制的氧空位促进纳米套接字Cu/钙钛矿异质结构上的CO 2 -到C 2+的转化。对于Cu/La 0.3-x Sr 0.6+x TiO 3-δ （x从0到0.3）的概念验证催化剂，其氧空位浓度随着A位价态的降低（或x值的增加）而可控地增加）。在流通池中，它们对C 2+的活性和选择性与氧空位浓度呈正相关。其中，氧空位最多的Cu/Sr 0.9 TiO 3-δ对C 2+显示出最佳的活性和选择性。并且相对于具有最小氧空位的Cu/La 0.3 Sr 0.6 TiO 3-δ ，Cu/Sr 0.9 TiO 3-δ在C 2+的活性和选择性方面表现出显着的改进（高达2.4倍）。实验和理论计算表明，优化的性能可归因于氧空位提供的优点，包括加速电荷转移、增强反应物质的吸附/活化以及降低C─C耦合的能垒。此外，当在膜电极组件电解槽中进行探索时，Cu/Sr 0.9 TiO 3-δ催化剂表现出优异的活性、选择性（43.9%），并且在工业电流密度下对C 2 H 4具有稳定性，是CO 2转化为C 2 H 4的最有效的钙钛矿基催化剂。
更新日期：2024-03-13
中文翻译：
通过 A 位价控制的氧空位促进纳米插座铜/钙钛矿异质结构上的 CO2 电还原
尽管具有令人着迷的潜力，但用于CO 2电还原（CO 2 RR）的纳米套接字Cu/钙钛矿异质结构仍处于起步阶段，并且缺乏对其CO 2 RR性能的合理优化。在此，报道了一种有效的策略，通过A位价控制的氧空位促进纳米套接字Cu/钙钛矿异质结构上的CO 2 -到C 2+的转化。对于Cu/La 0.3-x Sr 0.6+x TiO 3-δ （x从0到0.3）的概念验证催化剂，其氧空位浓度随着A位价态的降低（或x值的增加）而可控地增加）。在流通池中，它们对C 2+的活性和选择性与氧空位浓度呈正相关。其中，氧空位最多的Cu/Sr 0.9 TiO 3-δ对C 2+显示出最佳的活性和选择性。并且相对于具有最小氧空位的Cu/La 0.3 Sr 0.6 TiO 3-δ ，Cu/Sr 0.9 TiO 3-δ在C 2+的活性和选择性方面表现出显着的改进（高达2.4倍）。实验和理论计算表明，优化的性能可归因于氧空位提供的优点，包括加速电荷转移、增强反应物质的吸附/活化以及降低C─C耦合的能垒。此外，当在膜电极组件电解槽中进行探索时，Cu/Sr 0.9 TiO 3-δ催化剂表现出优异的活性、选择性（43.9%），并且在工业电流密度下对C 2 H 4具有稳定性，是CO 2转化为C 2 H 4的最有效的钙钛矿基催化剂。
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