Tuning chemical environment and synergistic relay reaction to promote higher alcohols synthesis via syngas conversion

Tingting Qin; Tiejun Lin; Xingzhen Qi; Caiqi Wang; Liusha Li; Zhiyong Tang; Liangshu Zhong; Yuhan Sun

doi:10.1016/j.apcatb.2020.119840

Tuning chemical environment and synergistic relay reaction to promote higher alcohols synthesis via syngas conversion

Tingting Qin
, Tiejun Lin
, Xingzhen Qi
, Caiqi Wang
, Liusha Li
, Zhiyong Tang
, Liangshu Zhong
, Yuhan Sun

Surface Chemistry & Catalysis Group

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

71 Scopus citations

Abstract

Higher alcohols synthesis (HAS) from syngas with high selectivity attracts great attention but remains challenging. Herein, we reported an effective strategy by tuning chemical environment and synergistic relay reaction to promote the production of higher alcohols. CO insertion rate was greatly enhanced by introducing Rh or Ru component to CoMn oxides. The catalytic activity and oxygenates selectivity increased dramatically over the as-obtained Rh-CoMn or Ru-CoMn catalyst, while the fraction of C₂₊OH in oxygenates maintained >92 %. Multiple studies demonstrated the highly dispersed Rh^δ+ or Ru^δ+ species not only effectively tuned the chemical environment and facilitated the stable existence of Co₂C, but also catalyzed the coupling of syngas and in-situ generated olefins to produce extra oxygenates via hydroformylation route. The synergistic effect of Co⁰, Co₂C and Rh^δ+ (or Ru^δ+) species, as well as the promotional effect of olefins relay reaction contributed to the enhancement in both higher alcohols selectivity and CO conversion.

Original language	English
Article number	119840
Journal	Applied Catalysis B: Environmental
Volume	285
DOIs	https://doi.org/10.1016/j.apcatb.2020.119840
State	Published - May 15 2021

Funding

This work was financially supported by Natural Science Foundation of China ( 91945301 , 22072177 , 21776296 and 21703278 ), the National Key R&D Program of China ( 2017YFB0602202 ), Program of Shanghai Academic/Technology Research Leader ( 20XD1404000 ), Key Research Program of Frontier Sciences, CAS (Grant No. QYZDB-SSW-SLH035 ), the “Transformational Technologies for Clean Energy and Demonstration” , Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No. XDA21020600 ), Youth Innovation Promotion Association of CAS and Xin Rui Excellent Young Talents Program of SARI ( E054881ZZ1 ).

Keywords

CoC
Higher alcohols
Hydroformylation
Synergistic effect
Syngas conversion

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title = "Tuning chemical environment and synergistic relay reaction to promote higher alcohols synthesis via syngas conversion",

abstract = "Higher alcohols synthesis (HAS) from syngas with high selectivity attracts great attention but remains challenging. Herein, we reported an effective strategy by tuning chemical environment and synergistic relay reaction to promote the production of higher alcohols. CO insertion rate was greatly enhanced by introducing Rh or Ru component to CoMn oxides. The catalytic activity and oxygenates selectivity increased dramatically over the as-obtained Rh-CoMn or Ru-CoMn catalyst, while the fraction of C2+OH in oxygenates maintained >92 \%. Multiple studies demonstrated the highly dispersed Rhδ+ or Ruδ+ species not only effectively tuned the chemical environment and facilitated the stable existence of Co2C, but also catalyzed the coupling of syngas and in-situ generated olefins to produce extra oxygenates via hydroformylation route. The synergistic effect of Co0, Co2C and Rhδ+ (or Ruδ+) species, as well as the promotional effect of olefins relay reaction contributed to the enhancement in both higher alcohols selectivity and CO conversion.",

keywords = "CoC, Higher alcohols, Hydroformylation, Synergistic effect, Syngas conversion",

author = "Tingting Qin and Tiejun Lin and Xingzhen Qi and Caiqi Wang and Liusha Li and Zhiyong Tang and Liangshu Zhong and Yuhan Sun",

note = "Publisher Copyright: {\textcopyright} 2020 Elsevier B.V.",

year = "2021",

month = may,

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doi = "10.1016/j.apcatb.2020.119840",

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T1 - Tuning chemical environment and synergistic relay reaction to promote higher alcohols synthesis via syngas conversion

AU - Qin, Tingting

AU - Lin, Tiejun

AU - Qi, Xingzhen

AU - Wang, Caiqi

AU - Li, Liusha

AU - Tang, Zhiyong

AU - Zhong, Liangshu

AU - Sun, Yuhan

PY - 2021/5/15

Y1 - 2021/5/15

N2 - Higher alcohols synthesis (HAS) from syngas with high selectivity attracts great attention but remains challenging. Herein, we reported an effective strategy by tuning chemical environment and synergistic relay reaction to promote the production of higher alcohols. CO insertion rate was greatly enhanced by introducing Rh or Ru component to CoMn oxides. The catalytic activity and oxygenates selectivity increased dramatically over the as-obtained Rh-CoMn or Ru-CoMn catalyst, while the fraction of C2+OH in oxygenates maintained >92 %. Multiple studies demonstrated the highly dispersed Rhδ+ or Ruδ+ species not only effectively tuned the chemical environment and facilitated the stable existence of Co2C, but also catalyzed the coupling of syngas and in-situ generated olefins to produce extra oxygenates via hydroformylation route. The synergistic effect of Co0, Co2C and Rhδ+ (or Ruδ+) species, as well as the promotional effect of olefins relay reaction contributed to the enhancement in both higher alcohols selectivity and CO conversion.

AB - Higher alcohols synthesis (HAS) from syngas with high selectivity attracts great attention but remains challenging. Herein, we reported an effective strategy by tuning chemical environment and synergistic relay reaction to promote the production of higher alcohols. CO insertion rate was greatly enhanced by introducing Rh or Ru component to CoMn oxides. The catalytic activity and oxygenates selectivity increased dramatically over the as-obtained Rh-CoMn or Ru-CoMn catalyst, while the fraction of C2+OH in oxygenates maintained >92 %. Multiple studies demonstrated the highly dispersed Rhδ+ or Ruδ+ species not only effectively tuned the chemical environment and facilitated the stable existence of Co2C, but also catalyzed the coupling of syngas and in-situ generated olefins to produce extra oxygenates via hydroformylation route. The synergistic effect of Co0, Co2C and Rhδ+ (or Ruδ+) species, as well as the promotional effect of olefins relay reaction contributed to the enhancement in both higher alcohols selectivity and CO conversion.

KW - CoC

KW - Higher alcohols

KW - Hydroformylation

KW - Synergistic effect

KW - Syngas conversion

UR - https://www.scopus.com/pages/publications/85098569090

U2 - 10.1016/j.apcatb.2020.119840

DO - 10.1016/j.apcatb.2020.119840

M3 - Article

AN - SCOPUS:85098569090

SN - 0926-3373

VL - 285

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

M1 - 119840

ER -

Tuning chemical environment and synergistic relay reaction to promote higher alcohols synthesis via syngas conversion

Abstract

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Keywords

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