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Achieving efficient and robust catalytic reforming on dual-sites of Cu species

Catalytic reforming provides a practical technique for on-board hydrogen production in fuel cell applications. The high energy density, easy transportation and non-toxicity of biomass-derived dimethyl ether (bio-DME) offer potential to replace methanol for on-board steam reforming (SR). Presently, t...

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Autores principales: Ma, Kui, Tian, Ye, Zhao, Zhi-Jian, Cheng, Qingpeng, Ding, Tong, Zhang, Jing, Zheng, Lirong, Jiang, Zheng, Abe, Takayuki, Tsubaki, Noritatsu, Gong, Jinlong, Li, Xingang
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Royal Society of Chemistry 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6429598/
https://www.ncbi.nlm.nih.gov/pubmed/30996972
http://dx.doi.org/10.1039/c9sc00015a
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author Ma, Kui
Tian, Ye
Zhao, Zhi-Jian
Cheng, Qingpeng
Ding, Tong
Zhang, Jing
Zheng, Lirong
Jiang, Zheng
Abe, Takayuki
Tsubaki, Noritatsu
Gong, Jinlong
Li, Xingang
author_facet Ma, Kui
Tian, Ye
Zhao, Zhi-Jian
Cheng, Qingpeng
Ding, Tong
Zhang, Jing
Zheng, Lirong
Jiang, Zheng
Abe, Takayuki
Tsubaki, Noritatsu
Gong, Jinlong
Li, Xingang
author_sort Ma, Kui
collection PubMed
description Catalytic reforming provides a practical technique for on-board hydrogen production in fuel cell applications. The high energy density, easy transportation and non-toxicity of biomass-derived dimethyl ether (bio-DME) offer potential to replace methanol for on-board steam reforming (SR). Presently, the reaction mechanism over conventional Cu-based SR catalysts remains elusive, limiting the rational design of highly efficient reforming systems. Herein, we build a catalytic system for bio-DME SR with dual-sites of Cu species, i.e., Cu(+) and Cu(0) sites, and achieve a record-high H(2) production rate of 1145 mol kg(cat)(–1) h(–1). Via regulating the ratios of the dual-sites of Cu, we clearly describe molecular understandings on SR. And we discover that the substantially boosted activity is induced by a new Cu(+)-determined reaction path substituting the conventional Cu(0)-determined path. Intrinsically, Cu(2)O can act as a physical spacer and hydroxyl consumer to suppress the aggregation of metallic Cu species in SR. Due to the unique structure of metallic Cu surrounded by Cu(2)O, the catalyst exhibits robust catalytic performance even after severe thermal treatment. These findings open a new avenue for designing efficient catalytic reforming systems with commercial potential.
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spelling pubmed-64295982019-04-17 Achieving efficient and robust catalytic reforming on dual-sites of Cu species Ma, Kui Tian, Ye Zhao, Zhi-Jian Cheng, Qingpeng Ding, Tong Zhang, Jing Zheng, Lirong Jiang, Zheng Abe, Takayuki Tsubaki, Noritatsu Gong, Jinlong Li, Xingang Chem Sci Chemistry Catalytic reforming provides a practical technique for on-board hydrogen production in fuel cell applications. The high energy density, easy transportation and non-toxicity of biomass-derived dimethyl ether (bio-DME) offer potential to replace methanol for on-board steam reforming (SR). Presently, the reaction mechanism over conventional Cu-based SR catalysts remains elusive, limiting the rational design of highly efficient reforming systems. Herein, we build a catalytic system for bio-DME SR with dual-sites of Cu species, i.e., Cu(+) and Cu(0) sites, and achieve a record-high H(2) production rate of 1145 mol kg(cat)(–1) h(–1). Via regulating the ratios of the dual-sites of Cu, we clearly describe molecular understandings on SR. And we discover that the substantially boosted activity is induced by a new Cu(+)-determined reaction path substituting the conventional Cu(0)-determined path. Intrinsically, Cu(2)O can act as a physical spacer and hydroxyl consumer to suppress the aggregation of metallic Cu species in SR. Due to the unique structure of metallic Cu surrounded by Cu(2)O, the catalyst exhibits robust catalytic performance even after severe thermal treatment. These findings open a new avenue for designing efficient catalytic reforming systems with commercial potential. Royal Society of Chemistry 2019-01-23 /pmc/articles/PMC6429598/ /pubmed/30996972 http://dx.doi.org/10.1039/c9sc00015a Text en This journal is © The Royal Society of Chemistry 2019 https://creativecommons.org/licenses/by-nc/3.0/This article is freely available. This article is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported Licence (CC BY-NC 3.0)
spellingShingle Chemistry
Ma, Kui
Tian, Ye
Zhao, Zhi-Jian
Cheng, Qingpeng
Ding, Tong
Zhang, Jing
Zheng, Lirong
Jiang, Zheng
Abe, Takayuki
Tsubaki, Noritatsu
Gong, Jinlong
Li, Xingang
Achieving efficient and robust catalytic reforming on dual-sites of Cu species
title Achieving efficient and robust catalytic reforming on dual-sites of Cu species
title_full Achieving efficient and robust catalytic reforming on dual-sites of Cu species
title_fullStr Achieving efficient and robust catalytic reforming on dual-sites of Cu species
title_full_unstemmed Achieving efficient and robust catalytic reforming on dual-sites of Cu species
title_short Achieving efficient and robust catalytic reforming on dual-sites of Cu species
title_sort achieving efficient and robust catalytic reforming on dual-sites of cu species
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6429598/
https://www.ncbi.nlm.nih.gov/pubmed/30996972
http://dx.doi.org/10.1039/c9sc00015a
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