Filling COFs with bimetallic nanoclusters for CO2-to-alcohols conversion with H2O oxidation

Yamei Huang; Peiyao Du; Wen Xiong Shi; Ye Wang; Shuang Yao; Zhi Ming Zhang; Tong Bu Lu; Xiaoquan Lu

doi:10.1016/j.apcatb.2021.120001

Filling COFs with bimetallic nanoclusters for CO₂-to-alcohols conversion with H₂O oxidation

Yamei Huang
, Peiyao Du
, Wen Xiong Shi
, Ye Wang
, Shuang Yao
, Zhi Ming Zhang
, Tong Bu Lu
, Xiaoquan Lu

Tianjin University
Tianjin University of Technology

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

108 Scopus citations

Abstract

Solar-driven CO₂ reduction with H₂O oxidation into liquid fuels is highly desirable for sustainable carbon cycle to achieve carbon neutral, but represents a great challenge for artificial photosynthesis. Herein, bimetallic PdIn nanoclusters are confined in a photosensitizing covalent organic framework (N₃-COF) to facilely construct Pd_xIn_y@N₃-COF composites (x:y = 1:0, 0:1, 1:2, 1:1, 2:1). The resulting PdIn@N₃-COF exhibits excellent activity for CO₂ photoreduction with H₂O oxidation as the H⁺ and e⁻ source, showing a record-high total yield of 798 μmol g^-1 for producing CH₃OH (74 %) and CH₃CH₂OH (26 %) among the framework materials. The synergy in both the bimetallic nanocluster and cluster@N₃-COF contributes greatly to C[sbnd]C coupling and interfacial charge transfer, thus achieving excellent activity for conversion of CO₂ to C₁/C₂ alcohols on the non-copper catalysts. This work highlights the amazing potential for constructing bimetallic nanocluster@photosensitizing supports to produce alcohols in artificial photosynthesis with H₂O oxidation.

Original language	English
Article number	120001
Journal	Applied Catalysis B: Environmental
Volume	288
DOIs	https://doi.org/10.1016/j.apcatb.2021.120001
State	Published - 5 Jul 2021
Externally published	Yes

Keywords

Bimetallic nanoclusters
CO photoreduction
Covalent organic frameworks
HO oxidation

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10.1016/j.apcatb.2021.120001

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title = "Filling COFs with bimetallic nanoclusters for CO2-to-alcohols conversion with H2O oxidation",

abstract = "Solar-driven CO2 reduction with H2O oxidation into liquid fuels is highly desirable for sustainable carbon cycle to achieve carbon neutral, but represents a great challenge for artificial photosynthesis. Herein, bimetallic PdIn nanoclusters are confined in a photosensitizing covalent organic framework (N3-COF) to facilely construct PdxIny@N3-COF composites (x:y = 1:0, 0:1, 1:2, 1:1, 2:1). The resulting PdIn@N3-COF exhibits excellent activity for CO2 photoreduction with H2O oxidation as the H+ and e− source, showing a record-high total yield of 798 μmol g-1 for producing CH3OH (74 \%) and CH3CH2OH (26 \%) among the framework materials. The synergy in both the bimetallic nanocluster and cluster@N3-COF contributes greatly to C[sbnd]C coupling and interfacial charge transfer, thus achieving excellent activity for conversion of CO2 to C1/C2 alcohols on the non-copper catalysts. This work highlights the amazing potential for constructing bimetallic nanocluster@photosensitizing supports to produce alcohols in artificial photosynthesis with H2O oxidation.",

keywords = "Bimetallic nanoclusters, CO photoreduction, Covalent organic frameworks, HO oxidation",

author = "Yamei Huang and Peiyao Du and Shi, \{Wen Xiong\} and Ye Wang and Shuang Yao and Zhang, \{Zhi Ming\} and Lu, \{Tong Bu\} and Xiaoquan Lu",

note = "Publisher Copyright: {\textcopyright} 2021 Elsevier B.V.",

year = "2021",

month = jul,

day = "5",

doi = "10.1016/j.apcatb.2021.120001",

language = "英语",

volume = "288",

journal = "Applied Catalysis B: Environmental",

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TY - JOUR

T1 - Filling COFs with bimetallic nanoclusters for CO2-to-alcohols conversion with H2O oxidation

AU - Huang, Yamei

AU - Du, Peiyao

AU - Shi, Wen Xiong

AU - Wang, Ye

AU - Yao, Shuang

AU - Zhang, Zhi Ming

AU - Lu, Tong Bu

AU - Lu, Xiaoquan

PY - 2021/7/5

Y1 - 2021/7/5

N2 - Solar-driven CO2 reduction with H2O oxidation into liquid fuels is highly desirable for sustainable carbon cycle to achieve carbon neutral, but represents a great challenge for artificial photosynthesis. Herein, bimetallic PdIn nanoclusters are confined in a photosensitizing covalent organic framework (N3-COF) to facilely construct PdxIny@N3-COF composites (x:y = 1:0, 0:1, 1:2, 1:1, 2:1). The resulting PdIn@N3-COF exhibits excellent activity for CO2 photoreduction with H2O oxidation as the H+ and e− source, showing a record-high total yield of 798 μmol g-1 for producing CH3OH (74 %) and CH3CH2OH (26 %) among the framework materials. The synergy in both the bimetallic nanocluster and cluster@N3-COF contributes greatly to C[sbnd]C coupling and interfacial charge transfer, thus achieving excellent activity for conversion of CO2 to C1/C2 alcohols on the non-copper catalysts. This work highlights the amazing potential for constructing bimetallic nanocluster@photosensitizing supports to produce alcohols in artificial photosynthesis with H2O oxidation.

AB - Solar-driven CO2 reduction with H2O oxidation into liquid fuels is highly desirable for sustainable carbon cycle to achieve carbon neutral, but represents a great challenge for artificial photosynthesis. Herein, bimetallic PdIn nanoclusters are confined in a photosensitizing covalent organic framework (N3-COF) to facilely construct PdxIny@N3-COF composites (x:y = 1:0, 0:1, 1:2, 1:1, 2:1). The resulting PdIn@N3-COF exhibits excellent activity for CO2 photoreduction with H2O oxidation as the H+ and e− source, showing a record-high total yield of 798 μmol g-1 for producing CH3OH (74 %) and CH3CH2OH (26 %) among the framework materials. The synergy in both the bimetallic nanocluster and cluster@N3-COF contributes greatly to C[sbnd]C coupling and interfacial charge transfer, thus achieving excellent activity for conversion of CO2 to C1/C2 alcohols on the non-copper catalysts. This work highlights the amazing potential for constructing bimetallic nanocluster@photosensitizing supports to produce alcohols in artificial photosynthesis with H2O oxidation.

KW - Bimetallic nanoclusters

KW - CO photoreduction

KW - Covalent organic frameworks

KW - HO oxidation

UR - https://www.scopus.com/pages/publications/85101599813

U2 - 10.1016/j.apcatb.2021.120001

DO - 10.1016/j.apcatb.2021.120001

M3 - 文章

AN - SCOPUS:85101599813

SN - 0926-3373

VL - 288

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

M1 - 120001

ER -

Filling COFs with bimetallic nanoclusters for CO₂-to-alcohols conversion with H₂O oxidation

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Keywords

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