理性调控铂d电子显著提升液态有机氢载体催化脱氢性能

Chao Sun; Tianzuo Wang; Ruijie Gao; Xiaoyang Liu; Kang Xue; Chengxiang Shi; Xiangwen Zhang; Lun Pan; Ji-Jun Zou

doi:10.1016/j.eng.2025.07.045

工程（英文） ›› 2026, Vol. 57 ›› Issue (2) : 217 -226. DOI: 10.1016/j.eng.2025.07.045

研究论文

理性调控铂d电子显著提升液态有机氢载体催化脱氢性能

Chao Sun ^a^,^b^,^d ,
Tianzuo Wang ^a^,^b^,^d ,
Ruijie Gao ^a^,^b^,^c^,^d ,
Xiaoyang Liu ^d ,
Kang Xue ^a^,^b^,^c^,^d ,
Chengxiang Shi ^a^,^b^,^d ,
Xiangwen Zhang ^a^,^b^,^c^,^d ,
Lun Pan ^a^,^b^,^c^,^d^,^* ,
Ji-Jun Zou ^a^,^b^,^c^,^d^,^*

作者信息 +

Rational Modulation of Pt d Electrons to Significantly Enhance the Catalytic Dehydrogenation Performance of Liquid Organic Hydrogen Carriers

Chao Sun ^a^,^b^,^d ,
Tianzuo Wang ^a^,^b^,^d ,
Ruijie Gao ^a^,^b^,^c^,^d ,
Xiaoyang Liu ^d ,
Kang Xue ^a^,^b^,^c^,^d ,
Chengxiang Shi ^a^,^b^,^d ,
Xiangwen Zhang ^a^,^b^,^c^,^d ,
Lun Pan ^a^,^b^,^c^,^d^,^* ,
Ji-Jun Zou ^a^,^b^,^c^,^d^,^*

Author information +

文章历史 +

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摘要

理解液态有机氢载体脱氢反应的本征特性颇具挑战性，这源于电子效应与几何效应的协同影响。本研究构建了具有相似铂粒径（约1.7 nm）的系列Pt/MOx催化剂（其中MOx为CeO2、MgO、ZrO2、TiO2、Al2O3或SiO2），旨在探究由金属-载体相互作用调控的铂电子结构对液态有机氢载体催化脱氢反应的影响。实验结果表明，不同载体上铂d电子含量与催化脱氢转化频率之间呈现火山型关联。其中，Pt/MgO催化剂表现出最优脱氢活性。当d电子含量降低时，Pt/MgO催化剂增强了Pt-C键的成键轨道占据特性，促使六氢单苄基甲苯（MBT）稳定吸附，进而促进后续C-H键断裂。该研究为通过调控铂位点d电子密度理性设计高效脱氢催化剂提供了新思路。

Abstract

Understanding the intrinsic features of dehydrogenation reactions of liquid organic hydrogen carriers (LOHCs) is a formidable challenge due to the combined impact of electronic and geometric effects. Herein, we constructed a series of Pt/MO_x catalysts (CeO₂, MgO, ZrO₂, TiO₂, Al₂O₃, or SiO₂) with similar sizes of Pt (∼1.7 nm) to investigate the effects of Pt electron structures (tuned by electronic metal-support interactions) on the catalytic dehydrogenation of LOHCs. The results revealed a volcano-shaped correlation between Pt d electrons on different supports and the turnover frequency of catalytic dehydrogenation. Importantly, the Pt/MgO catalyst exhibited the highest dehydrogenation activity. With decreasing d electron content, Pt/MgO increases the bonding orbital dominance of Pt-C bonds and leads to stable adsorption of H6-monobenzyltoluene (MBT), which facilitates subsequent C-H bond scission. This study offers insight for the strategic development of high-efficiency dehydrogenation catalysts via d electron density modulation of Pt sites.

关键词

Key words

Pt nanoparticles / Liquid organic hydrogen carriers / Dehydrogenation reaction / d electron

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Chao Sun,Tianzuo Wang,Ruijie Gao,Xiaoyang Liu,Kang Xue,Chengxiang Shi,Xiangwen Zhang,Lun Pan,Ji-Jun Zou. 理性调控铂d电子显著提升液态有机氢载体催化脱氢性能[J]. 工程（英文）, 2026, 57(2): 217-226 DOI:10.1016/j.eng.2025.07.045