Huang Jialu, Deng Chengwei, Liu Yue, Han Tingting, Ji Feng, Zhang Yuehua, Lu Hongbin, Hua Ping, Zhang Bowei, Qian Tao, Yuan Xiaolei, Yang Yaoyue, Yao Yong
School of Chemistry and Chemical Engineering, Nantong University, Nantong 226019, China.
State Key Laboratory of Space Power-Sources Technology, Shanghai Institute of Space Power-Sources, Shanghai 200245, China.
J Colloid Interface Sci. 2022 Apr;611:327-335. doi: 10.1016/j.jcis.2021.12.103. Epub 2021 Dec 20.
Palladium (Pd) is supposed to be one of the most promising catalytic metals towards ethanol (CHOH) oxidation reaction (EOR). However, Pd electrocatalysts easily suffer from the poisoning of the intermediates (especially CO), resulting in the quick decay of EOR catalysis. Herein, inspired by the Brønsted-Lowry acid-base theory, a "attraction-repulsion" concept is proposed to guide the surface structure engineering toward EOR catalysts. Specifically, we induce Bi(OH) species as Brønsted base onto PdBi nanoplates to effectively repel the adsorption of CO intermediates. The PdBi-Bi(OH) nanoplates show an impressive mass activity of 4.46 A mg during the EOR catalysis and keep excellent stability. Both the stability and enhanced performance are attributed by the interfacial Brønsted base Bi(OH) which can selectively attract and repel reactants and intermediates, as evidenced from in situ measurements and theoretical views.
钯（Pd）被认为是对乙醇（CH₃OH）氧化反应（EOR）最具潜力的催化金属之一。然而，钯电催化剂很容易受到中间体（尤其是CO）的毒化，导致EOR催化作用迅速衰减。在此，受布朗斯特-劳里酸碱理论的启发，提出了一种“吸引-排斥”概念来指导EOR催化剂的表面结构工程。具体而言，我们将Bi(OH)物种作为布朗斯特碱引入到PdBi纳米片上，以有效排斥CO中间体的吸附。PdBi-Bi(OH)纳米片在EOR催化过程中表现出令人印象深刻的4.46 A mg的质量活性，并保持优异的稳定性。稳定性和性能的增强都归因于界面布朗斯特碱Bi(OH)，它可以选择性地吸引和排斥反应物及中间体，原位测量和理论观点都证明了这一点。
