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用于增强将CO电还原为C的钙钛矿套接亚3纳米铜

Perovskite-Socketed Sub-3 nm Copper for Enhanced CO Electroreduction to C.

作者信息

Li Yuxi, Liu Fuzhu, Chen Zitao, Shi Lei, Zhang Zhenbao, Gong Yue, Zhang Yu, Tian Xuezeng, Zhang Yu, Qiu Xiaoyu, Ding Xiangdong, Bai Xuedong, Jiang Heqing, Zhu Yongfa, Zhu Jiawei

机构信息

Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi, 214122, China.

State Key Laboratory for Mechanical Behavior of Materials, Xi'an Jiaotong University, Xi'an, 710049, China.

出版信息

Adv Mater. 2022 Nov;34(44):e2206002. doi: 10.1002/adma.202206002. Epub 2022 Sep 30.

Abstract

In situ socketing metal nanoparticles onto perovskite oxides has shown great potential in heterogeneous catalysis, but its employment in boosting ambient CO electroreduction (CER) is unexplored. Here, a CER catalyst of perovskite-socketed sub-3 nm Cu equipped with strong metal-support interactions (SMSIs) is constructed to promote efficient and stable CO -to-C conversion. For such a catalyst, plentiful sub-3 nm ellipsoid Cu particles are homogeneously and epitaxially anchored on the perovskite backbones, with concomitant creation of significant SMSIs. These SMSIs are able to not only modulate electronic structure of active Cu and facilitate adsorption/activation of key intermediates, but also to strengthen perovskite-Cu adhesion and intensify resistance to structural degradation. Beneficial from these advantageous merits, when evaluated in CER, it performs comparably to or better than most reported Cu-based heteronanostructures. Relative to a physical-mixture counterpart, it features marked improvements (up to 6.2 folds) in activity and selectivity for C , together with greatly boosted stability (>80 h). This work gives a new avenue to rationally design more advanced Cu-based heteronanostructures for CER.

摘要

在钙钛矿氧化物上原位套接金属纳米颗粒在多相催化中已显示出巨大潜力,但尚未探索其在促进常温常压下的CO电还原(CER)中的应用。在此,构建了一种具有强金属-载体相互作用(SMSIs)的钙钛矿套接亚3纳米铜的CER催化剂,以促进高效且稳定的CO到C的转化。对于这种催化剂,大量亚3纳米的椭球形铜颗粒均匀且外延地锚定在钙钛矿骨架上,同时产生显著的SMSIs。这些SMSIs不仅能够调节活性铜的电子结构并促进关键中间体的吸附/活化,还能增强钙钛矿与铜的附着力并增强对结构降解的抗性。受益于这些有利特性,在CER评估中,它的表现与大多数已报道的铜基异质纳米结构相当或更好。相对于物理混合的对应物,它在C的活性和选择性方面有显著提高(高达6.2倍),同时稳定性大大提高(>80小时)。这项工作为合理设计用于CER的更先进的铜基异质纳米结构提供了一条新途径。

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