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Phase-Dependent Electrocatalytic CO2 Reduction on Pd3Bi Nanocrystals
Angewandte Chemie International Edition ( IF 16.6 ) Pub Date : 2021-08-11 , DOI: 10.1002/anie.202109288
Lin Jia 1 , Mingzi Sun 2 , Jie Xu 1 , Xuan Zhao 1 , Rui Zhou 1 , Binbin Pan 1 , Lu Wang 1 , Na Han 1 , Bolong Huang 2 , Yanguang Li 1
Affiliation  

Alloying is a general strategy for modulating the electronic structures of catalyst materials. Compared to more common solid–solution alloys, intermetallic alloys feature well-defined atomic arrangements and provide the unique platform for studying the structure-performance correlations. It is, unfortunately, synthetically challenging to prepare the nanostructures of intermetallic alloys for catalysis research. In this contribution, we prepare intermetallic Pd3Bi nanocrystals of a uniform size via a facile solvothermal method. These nanocrystals can phase-transform into solid solution alloy via thermal annealing while retaining a similar composition and size. In 0.1 M KHCO3 aqueous solution, the intermetallic Pd3Bi can selectively reduce CO2 to formate with high selectivity (≈100 %) and stability even at <-0.35 V versus reversible hydrogen electrode, whereas the solid solution alloy has limited formate selectivity of <60 %. Such unique phase-dependence is understood via theoretical simulations showing that the crystallographic ordering of Pd and Bi atoms within intermetallic alloys can suppress CO poisoning and enhance the *OCHO adsorption during electrochemical CO2 reduction to formate.

中文翻译:

Pd3Bi 纳米晶体上的相依赖电催化 CO2 还原

合金化是调节催化剂材料电子结构的通用策略。与更常见的固溶合金相比,金属间合金具有明确的原子排列,并为研究结构-性能相关性提供了独特的平台。不幸的是,制备用于催化研究的金属间合金纳米结构在综合方面具有挑战性。在这一贡献中,我们通过简便的溶剂热法制备了尺寸均匀的金属间 Pd 3 Bi 纳米晶体。这些纳米晶体可以通过热退火相转变为固溶体合金,同时保持相似的成分和尺寸。在0.1 M KHCO 3水溶液中,金属间化合物Pd 3 Bi可以选择性还原CO 2与可逆氢电极相比,即使在 <-0.35 V 下也具有高选择性 (≈100%) 和稳定性,而固溶体合金的甲酸盐选择性有限,<60%。这种独特的相依赖性是通过理论模拟来理解的,该理论表明金属间合金中 Pd 和 Bi 原子的晶体排列可以抑制 CO 中毒并增强在电化学 CO 2还原为甲酸盐过程中的 *OCHO 吸附。
更新日期:2021-09-20
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