Exploiting quasi-one-dimensional confinement for proficient hydrogen production from formic acid at room temperature

doi:10.1016/j.jechem.2020.02.040

能源化学(英文版) ›› 2020, Vol. 49 ›› Issue (10): 205-213.DOI: 10.1016/j.jechem.2020.02.040

Exploiting quasi-one-dimensional confinement for proficient hydrogen production from formic acid at room temperature

Tao Jiang, Peng Lu, Meng-Jiao Xu, Jian-Dong Lin, Yong-Mei Liu, Yong Cao, He-Yong He

Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials,Department of Chemistry,Fudan University,Shanghai 200433,China

收稿日期:2019-12-26 修回日期:2020-02-25 出版日期:2020-10-15 发布日期:2020-12-18
通讯作者: Yong-Mei Liu, Yong Cao
基金资助:
Financial support from NSF of China(21773033,21972024,91645201),Science & Technology Commission of Shanghai Municipality(19DZ2270100),and SINOPEC(X514005)is acknowledged.

Exploiting quasi-one-dimensional confinement for proficient hydrogen production from formic acid at room temperature

Tao Jiang, Peng Lu, Meng-Jiao Xu, Jian-Dong Lin, Yong-Mei Liu, Yong Cao, He-Yong He

Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials,Department of Chemistry,Fudan University,Shanghai 200433,China

Received:2019-12-26 Revised:2020-02-25 Online:2020-10-15 Published:2020-12-18
Contact: Yong-Mei Liu, Yong Cao
Supported by:
Financial support from NSF of China(21773033,21972024,91645201),Science & Technology Commission of Shanghai Municipality(19DZ2270100),and SINOPEC(X514005)is acknowledged.

摘要/Abstract

摘要： We describe herein that the quasi-one-dimensional confinement effect of functionalized nanoporous supports is particularly advantageous for boosting formic acid (FA) dehydrogenation efficiency over palladium nanoparticles (NPs).Benefiting from their unique structural merits that lead to significant lowering of the entropic barrier for FA activation,the Pd NPs interiorly located on the amino-modified MCM-41 offer the promise of more than an order of magnitude speedup of the initial activity in H₂ production from FA over their exterior analogs.Under mild and additive-free conditions,ultrafine Pd NPs confined in aminomodified MCM-41 channels exhibit an initial turnover frequency as high as 46,677 h^-1 and a turnover number up to 1,060,000 at 60℃.In conjunction with the enhancement and robust performance for efficient regeneration of FA via CO₂ hydrogenation,the presented approach greatly contributes to the development of FA-based hydrogen storage and related technologies as viable means of enabling sustainable future energy prospects.

关键词: Confinement effect, Formic acid, Heterogeneous catalysis, Hydrogen storage

Abstract: We describe herein that the quasi-one-dimensional confinement effect of functionalized nanoporous supports is particularly advantageous for boosting formic acid (FA) dehydrogenation efficiency over palladium nanoparticles (NPs).Benefiting from their unique structural merits that lead to significant lowering of the entropic barrier for FA activation,the Pd NPs interiorly located on the amino-modified MCM-41 offer the promise of more than an order of magnitude speedup of the initial activity in H₂ production from FA over their exterior analogs.Under mild and additive-free conditions,ultrafine Pd NPs confined in aminomodified MCM-41 channels exhibit an initial turnover frequency as high as 46,677 h^-1 and a turnover number up to 1,060,000 at 60℃.In conjunction with the enhancement and robust performance for efficient regeneration of FA via CO₂ hydrogenation,the presented approach greatly contributes to the development of FA-based hydrogen storage and related technologies as viable means of enabling sustainable future energy prospects.

Key words: Confinement effect, Formic acid, Heterogeneous catalysis, Hydrogen storage

Tao Jiang, Peng Lu, Meng-Jiao Xu, Jian-Dong Lin, Yong-Mei Liu, Yong Cao, He-Yong He. Exploiting quasi-one-dimensional confinement for proficient hydrogen production from formic acid at room temperature[J]. 能源化学(英文版), 2020, 49(10): 205-213.

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Exploiting quasi-one-dimensional confinement for proficient hydrogen production from formic acid at room temperature

Exploiting quasi-one-dimensional confinement for proficient hydrogen production from formic acid at room temperature

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