多孔 Pd3Pb 茂金属气凝胶中的低配位 Pd-Pb 位点可促进多元醇电化学氧化

IF 9.6 1区 化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Hui Fu, Zhen Huang, Ting Zhu*, Liheng Guan, Chih-Wen Pao, Wei-Hsiang Huang*, Nan Zhang* and Tianxi Liu*, 
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引用次数: 0

摘要

低配位位点能有效激活吸附剂,促进动力学速度较慢的电化学反应和多电子转移过程,但在电催化剂表面实现低配位位点的高暴露率仍具有挑战性。在此,我们首先介绍了通过动态重构策略合成具有低配位 Pd-Pb 位点的多孔 Pd3Pb 茂金属气凝胶(MAs),用于酒精氧化反应(AOR)。多孔 Pd3Pb MAs 在乙二醇氧化反应(EGOR)中具有较高的质量活性(1.63 A mgPd-1)、比活度(6.28 mA cm-2)和抗中毒特性,优于其他制备的催化剂。在乙醇氧化反应和甘油氧化反应中也观察到了同样的趋势。机理研究表明,具有低配位 Pd-Pb 位点的多孔 Pd3Pb MAs 可为乙二醇的吸附和活化提供更多的不饱和位点,并可降低 CH2OHCHO*、CH2OHCOO* 和 COOCOO*的反应能垒。这项工作为设计抗中毒 AOR 中的钯基催化剂探索了一个新思路。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Low-Coordinated Pd–Pb Sites in Porous Pd3Pb Metallene Aerogels Promote Polyalcohol Electrochemical Oxidation

Low-Coordinated Pd–Pb Sites in Porous Pd3Pb Metallene Aerogels Promote Polyalcohol Electrochemical Oxidation

Low-coordinated sites can effectively activate adsorbants and promote electrochemical reactions with slow kinetics and multielectron transfer processes, but achieving high exposure rates of low-coordinated sites on the electrocatalyst surface remains challenging. Herein, we first present the synthesis of the porous Pd3Pb metallene aerogels (MAs) with low-coordinated Pd–Pb sites through dynamic reconfiguration strategy for alcohol oxidation reaction (AOR). The porous Pd3Pb MAs possess high mass activity (1.63 A mgPd–1), specific activity (6.28 mA cm–2), and antipoisoning property in ethylene glycol oxidation reaction (EGOR), superior to other prepared catalysts. The same trend was observed in the ethanol oxidation reaction and glycerol oxidation reaction. Mechanism studies show that porous Pd3Pb MAs with low-coordinated Pd–Pb sites could provide more unsaturated sites for adsorption and activation of ethylene glycol, as well as lowering the reaction energy barriers of CH2OHCHO*, CH2OHCOO*, and COOCOO*. This work explored a novel idea for the design Pd-based catalysts in antipoisoned AOR.

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来源期刊
ACS Materials Letters
ACS Materials Letters MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
14.60
自引率
3.50%
发文量
261
期刊介绍: ACS Materials Letters is a journal that publishes high-quality and urgent papers at the forefront of fundamental and applied research in the field of materials science. It aims to bridge the gap between materials and other disciplines such as chemistry, engineering, and biology. The journal encourages multidisciplinary and innovative research that addresses global challenges. Papers submitted to ACS Materials Letters should clearly demonstrate the need for rapid disclosure of key results. The journal is interested in various areas including the design, synthesis, characterization, and evaluation of emerging materials, understanding the relationships between structure, property, and performance, as well as developing materials for applications in energy, environment, biomedical, electronics, and catalysis. The journal has a 2-year impact factor of 11.4 and is dedicated to publishing transformative materials research with fast processing times. The editors and staff of ACS Materials Letters actively participate in major scientific conferences and engage closely with readers and authors. The journal also maintains an active presence on social media to provide authors with greater visibility.
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