Construction of Synergistic Co and Cu Diatomic Sites for Enhanced Higher Alcohol Synthesis

Gaofeng Chen; Olga A. Syzgantseva; Maria A. Syzgantseva; Shuliang Yang; Guihua Yan; Li Peng; Changyan Cao; Wenxing Chen; Zhiwei Wang; Fengjuan Qin; Tingzhou Lei; Xianhai Zeng; Lu Lin; Weiguo Song; Buxing Han

doi:10.31635/ccschem.022.202201930

Construction of Synergistic Co and Cu Diatomic Sites for Enhanced Higher Alcohol Synthesis

Gaofeng Chen
, Olga A. Syzgantseva
, Maria A. Syzgantseva
, Shuliang Yang^*
, Guihua Yan
, Li Peng
, Changyan Cao
, Wenxing Chen^*
, Zhiwei Wang
, Fengjuan Qin
, Tingzhou Lei
, Xianhai Zeng^*
, Lu Lin
, Weiguo Song
, Buxing Han

^*Corresponding author for this work

School of Material Science and Engineering

Xiamen University
Lomonosov Moscow State University
Fujian Engineering and Research Center of Clean and High-valued Technologies for Biomass
CAS - Institute of Chemistry
University of Chinese Academy of Sciences
Henan University of Technology
Beijing Institute of Technology
Changzhou University

Research output: Contribution to journal › Article › peer-review

22 Citations (Scopus)

Abstract

Higher alcohol synthesis (HAS) from syngas could efficiently alleviate the dependence on the traditional fossil resources. However, it is still challenging to construct high-performance HAS catalysts with satisfying selectivity, space–time yield (STY), and stability. Herein, we designed a diatomic catalyst by anchoring Co and Cu sites onto a hierarchical porous N-doped carbon matrix (Co/Cu–N–C). The Co/Cu–N–C is efficient for HAS and is among the best catalysts reported. With a CO conversion of 81.7%, C₂₊OH selectivity could reach 58.5% with an outstanding C₂₊OH STY of 851.8 mg/g·h. We found that the N₄–Co₁ and Cu₁–N₄ showed an excellent synergistic effect. The adsorption of CO occurred on the Co site, and the surrounding nitrogen sites served as a hydrogen reservoir for the CO reduction reactions to form CH_xCo. Meanwhile, the Cu sites stabilized a CHO_Cu species to interact with CH_xCo, facilitating a barrier-free formation of C₂ species, which is responsible for the high selectivity of higher alcohols.

Original language	English
Pages (from-to)	851-864
Number of pages	14
Journal	CCS Chemistry
Volume	5
Issue number	4
DOIs	https://doi.org/10.31635/ccschem.022.202201930
Publication status	Published - Mar 2023

Keywords

carbon material
dual atomic catalyst
heterogeneous catalysis
higher alcohol synthesis
synergistic effect

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title = "Construction of Synergistic Co and Cu Diatomic Sites for Enhanced Higher Alcohol Synthesis",

abstract = "Higher alcohol synthesis (HAS) from syngas could efficiently alleviate the dependence on the traditional fossil resources. However, it is still challenging to construct high-performance HAS catalysts with satisfying selectivity, space–time yield (STY), and stability. Herein, we designed a diatomic catalyst by anchoring Co and Cu sites onto a hierarchical porous N-doped carbon matrix (Co/Cu–N–C). The Co/Cu–N–C is efficient for HAS and is among the best catalysts reported. With a CO conversion of 81.7\%, C2+OH selectivity could reach 58.5\% with an outstanding C2+OH STY of 851.8 mg/g·h. We found that the N4–Co1 and Cu1–N4 showed an excellent synergistic effect. The adsorption of CO occurred on the Co site, and the surrounding nitrogen sites served as a hydrogen reservoir for the CO reduction reactions to form CHxCo. Meanwhile, the Cu sites stabilized a CHOCu species to interact with CHxCo, facilitating a barrier-free formation of C2 species, which is responsible for the high selectivity of higher alcohols.",

keywords = "carbon material, dual atomic catalyst, heterogeneous catalysis, higher alcohol synthesis, synergistic effect",

author = "Gaofeng Chen and Syzgantseva, \{Olga A.\} and Syzgantseva, \{Maria A.\} and Shuliang Yang and Guihua Yan and Li Peng and Changyan Cao and Wenxing Chen and Zhiwei Wang and Fengjuan Qin and Tingzhou Lei and Xianhai Zeng and Lu Lin and Weiguo Song and Buxing Han",

year = "2023",

month = mar,

doi = "10.31635/ccschem.022.202201930",

language = "English",

volume = "5",

pages = "851--864",

journal = "CCS Chemistry",

issn = "2096-5745",

publisher = "Chinese Chemical Society",

number = "4",

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TY - JOUR

T1 - Construction of Synergistic Co and Cu Diatomic Sites for Enhanced Higher Alcohol Synthesis

AU - Chen, Gaofeng

AU - Syzgantseva, Olga A.

AU - Syzgantseva, Maria A.

AU - Yang, Shuliang

AU - Yan, Guihua

AU - Peng, Li

AU - Cao, Changyan

AU - Chen, Wenxing

AU - Wang, Zhiwei

AU - Qin, Fengjuan

AU - Lei, Tingzhou

AU - Zeng, Xianhai

AU - Lin, Lu

AU - Song, Weiguo

AU - Han, Buxing

PY - 2023/3

Y1 - 2023/3

N2 - Higher alcohol synthesis (HAS) from syngas could efficiently alleviate the dependence on the traditional fossil resources. However, it is still challenging to construct high-performance HAS catalysts with satisfying selectivity, space–time yield (STY), and stability. Herein, we designed a diatomic catalyst by anchoring Co and Cu sites onto a hierarchical porous N-doped carbon matrix (Co/Cu–N–C). The Co/Cu–N–C is efficient for HAS and is among the best catalysts reported. With a CO conversion of 81.7%, C2+OH selectivity could reach 58.5% with an outstanding C2+OH STY of 851.8 mg/g·h. We found that the N4–Co1 and Cu1–N4 showed an excellent synergistic effect. The adsorption of CO occurred on the Co site, and the surrounding nitrogen sites served as a hydrogen reservoir for the CO reduction reactions to form CHxCo. Meanwhile, the Cu sites stabilized a CHOCu species to interact with CHxCo, facilitating a barrier-free formation of C2 species, which is responsible for the high selectivity of higher alcohols.

AB - Higher alcohol synthesis (HAS) from syngas could efficiently alleviate the dependence on the traditional fossil resources. However, it is still challenging to construct high-performance HAS catalysts with satisfying selectivity, space–time yield (STY), and stability. Herein, we designed a diatomic catalyst by anchoring Co and Cu sites onto a hierarchical porous N-doped carbon matrix (Co/Cu–N–C). The Co/Cu–N–C is efficient for HAS and is among the best catalysts reported. With a CO conversion of 81.7%, C2+OH selectivity could reach 58.5% with an outstanding C2+OH STY of 851.8 mg/g·h. We found that the N4–Co1 and Cu1–N4 showed an excellent synergistic effect. The adsorption of CO occurred on the Co site, and the surrounding nitrogen sites served as a hydrogen reservoir for the CO reduction reactions to form CHxCo. Meanwhile, the Cu sites stabilized a CHOCu species to interact with CHxCo, facilitating a barrier-free formation of C2 species, which is responsible for the high selectivity of higher alcohols.

KW - carbon material

KW - dual atomic catalyst

KW - heterogeneous catalysis

KW - higher alcohol synthesis

KW - synergistic effect

UR - https://www.scopus.com/pages/publications/85159335894

U2 - 10.31635/ccschem.022.202201930

DO - 10.31635/ccschem.022.202201930

M3 - Article

AN - SCOPUS:85159335894

SN - 2096-5745

VL - 5

SP - 851

EP - 864

JO - CCS Chemistry

JF - CCS Chemistry

IS - 4

ER -

Construction of Synergistic Co and Cu Diatomic Sites for Enhanced Higher Alcohol Synthesis

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Keywords

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