Unveiling the pressure dependent deactivation mechanism of iridium-based catalysts for hydrogen production from formic acid aqueous solutions

被引:5
|
作者
Hao, Chuanqing [1 ]
Shen, Chengzhen [1 ]
Zhang, Yufan [1 ]
Liu, Jitian [2 ,3 ]
Zheng, Junrong [1 ]
机构
[1] Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, 292 Chengfu Rd, Beijing 100871, Peoples R China
[2] Shandong Univ, Dept Med Chem, Key Lab Chem Biol, Minist Educ, Jinan 250012, Shandong, Peoples R China
[3] Shandong Univ, Cheeloo Coll Med, Sch Pharmaceut Sci, NMPA Key Lab Technol Res & Evaluat Drug Prod, Jinan 250012, Shandong, Peoples R China
基金
美国国家科学基金会;
关键词
CO2; HYDROGENATION; DEHYDROGENATION; GENERATION; COMPLEXES; RUTHENIUM; STORAGE; DECOMPOSITION; LIGAND; CONSTANTS; DESIGN;
D O I
10.1016/j.ijhydene.2024.05.406
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Iridium-based catalysts exhibit promising potential for large-scaled hydrogen production from formic acid due to their high activity and stability in base-free aqueous solutions. However, their reactivity and lifetimes are highly pressure dependent, diminishing substantially under pressurized conditions necessary for the suppression of foam formation, imposing grand challenges for both fundamental understanding and practical applications. In this work, the deactivation mechanism is elucidated. Through a combination of experimental analyses and density functional theory (DFT) calculations, ligand dissociation and hydrogen poisoning are identified as the major deactivation pathways. A kinetic model resulted from the mechanism suggests that the deactivation is also inversely correlated to the catalyst concentration, verified by experiments. Built upon these deactivation insights, a 10-fold increase in reaction rate and a 2.5-fold increase in catalyst lifetime under pressure have been successfully realized by the addition of ligand that suppresses both ligand dissociation and hydrogen poisoning. These results not only address difficulties in practical applications but also offer valuable insights for future catalyst design.
引用
收藏
页码:744 / 754
页数:11
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