Steering the Selectivity of Carbon Dioxide Electroreduction from Single-Carbon to Multicarbon Products on Metal−Organic Frameworks via Facet Engineering

Pengyi Lu; Jia Lv; Yu Chen; Yangbo Ma; Yunhao Wang; Weichao Lyu; Jinli Yu; Jingwen Zhou; Jinwen Yin; Yuecheng Xiong; Guozhi Wang; Chongyi Ling; Shibo Xi; Daliang Zhang; Zhanxi Fan

doi:10.1021/acs.nanolett.3c04092

Steering the Selectivity of Carbon Dioxide Electroreduction from Single-Carbon to Multicarbon Products on Metal−Organic Frameworks via Facet Engineering

Pengyi Lu (Co-first Author)
, Jia Lv (Co-first Author)
, Yu Chen (Co-first Author)
, Yangbo Ma
, Yunhao Wang
, Weichao Lyu
, Jinli Yu
, Jingwen Zhou
, Jinwen Yin
, Yuecheng Xiong
, Guozhi Wang
, Chongyi Ling^*
, Shibo Xi^*
, Daliang Zhang
, Zhanxi Fan^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

39 Citations (Scopus)

20 Downloads (CityUHK Scholars)

Abstract

Although metal−organic frameworks (MOFs) have attracted more attention for the electrocatalytic CO₂ reduction reaction (CO₂RR), obtaining multicarbon products with a high Faradaic efficiency (FE) remains challenging, especially under neutral conditions. Here, we report the controlled synthesis of stable Cu(I) 5-mercapto-1-methyltetrazole framework (Cu-MMT) nanostructures with different facets by rationally modulating the reaction solvents. Significantly, Cu-MMT nanostructures with (001) facets are acquired using isopropanol as a solvent, which favor multicarbon production with an FE of 73.75% and a multicarbon:single-carbon ratio of 3.93 for CO₂RR in a neutral electrolyte. In sharp contrast, Cu-MMT nanostructures with (100) facets are obtained utilizing water, promoting single-carbon generation with an FE of 63.98% and a multicarbon: single-carbon ratio of only 0.18. Furthermore, this method can be extended to other Cu-MMT nanostructures with different facets in tuning the CO₂ reduction selectivity. This work opens up new opportunities for the highly selective and efficient CO₂ electroreduction to multicarbon products on MOFs via facet engineering. © 2024 American Chemical Society.

Original language	English
Pages (from-to)	1553-1562
Journal	Nano Letters
Volume	24
Issue number	5
Online published	24 Jan 2024
DOIs	https://doi.org/10.1021/acs.nanolett.3c04092
Publication status	Published - 7 Feb 2024

Funding

This work was supported by Grants 22175148 and 22005258 from the National Natural Science Foundation of China, Grant 21309322 from the Research Grants Council of Hong Kong, Grant JCYJ20220530140815035 from the Shenzhen Science and Technology Program, ITC via Hong Kong Branch of National Precious Metals Material Engineering Research Centre (NPMM), and Grants 9610480, 9610663, 9680301, and 7006007 from the City University of Hong Kong.

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 13 Climate Action

Research Keywords

carbon dioxide reduction reaction
electrocatalysis
facet engineering
metal−organic frameworks
multicarbon products

Publisher's Copyright Statement

COPYRIGHT TERMS OF DEPOSITED POSTPRINT FILE: This document is the Accepted Manuscript version of a Published Work that appeared in final form in Nano Letters, copyright © 2024 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.nanolett.3c04092.

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RGC-funded

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10.1021/acs.nanolett.3c04092

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Lu, P., Lv, J., Chen, Y., Ma, Y., Wang, Y., Lyu, W., Yu, J., Zhou, J., Yin, J., Xiong, Y., Wang, G., Ling, C., Xi, S., Zhang, D., & Fan, Z. (2024). Steering the Selectivity of Carbon Dioxide Electroreduction from Single-Carbon to Multicarbon Products on Metal−Organic Frameworks via Facet Engineering. Nano Letters, 24(5), 1553-1562. https://doi.org/10.1021/acs.nanolett.3c04092

@article{cb8299c06adc4790b559234604c2079e,

title = "Steering the Selectivity of Carbon Dioxide Electroreduction from Single-Carbon to Multicarbon Products on Metal−Organic Frameworks via Facet Engineering",

abstract = "Although metal−organic frameworks (MOFs) have attracted more attention for the electrocatalytic CO2 reduction reaction (CO2RR), obtaining multicarbon products with a high Faradaic efficiency (FE) remains challenging, especially under neutral conditions. Here, we report the controlled synthesis of stable Cu(I) 5-mercapto-1-methyltetrazole framework (Cu-MMT) nanostructures with different facets by rationally modulating the reaction solvents. Significantly, Cu-MMT nanostructures with (001) facets are acquired using isopropanol as a solvent, which favor multicarbon production with an FE of 73.75\% and a multicarbon:single-carbon ratio of 3.93 for CO2RR in a neutral electrolyte. In sharp contrast, Cu-MMT nanostructures with (100) facets are obtained utilizing water, promoting single-carbon generation with an FE of 63.98\% and a multicarbon: single-carbon ratio of only 0.18. Furthermore, this method can be extended to other Cu-MMT nanostructures with different facets in tuning the CO2 reduction selectivity. This work opens up new opportunities for the highly selective and efficient CO2 electroreduction to multicarbon products on MOFs via facet engineering. {\textcopyright} 2024 American Chemical Society.",

keywords = "carbon dioxide reduction reaction, electrocatalysis, facet engineering, metal−organic frameworks, multicarbon products",

author = "Pengyi Lu and Jia Lv and Yu Chen and Yangbo Ma and Yunhao Wang and Weichao Lyu and Jinli Yu and Jingwen Zhou and Jinwen Yin and Yuecheng Xiong and Guozhi Wang and Chongyi Ling and Shibo Xi and Daliang Zhang and Zhanxi Fan",

year = "2024",

month = feb,

day = "7",

doi = "10.1021/acs.nanolett.3c04092",

language = "English",

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Lu, P, Lv, J, Chen, Y, Ma, Y , Wang, Y, Lyu, W, Yu, J , Zhou, J , Yin, J , Xiong, Y , Wang, G, Ling, C, Xi, S, Zhang, D & Fan, Z 2024, 'Steering the Selectivity of Carbon Dioxide Electroreduction from Single-Carbon to Multicarbon Products on Metal−Organic Frameworks via Facet Engineering', Nano Letters, vol. 24, no. 5, pp. 1553-1562. https://doi.org/10.1021/acs.nanolett.3c04092

Steering the Selectivity of Carbon Dioxide Electroreduction from Single-Carbon to Multicarbon Products on Metal−Organic Frameworks via Facet Engineering. / Lu, Pengyi (Co-first Author); Lv, Jia (Co-first Author); Chen, Yu (Co-first Author) et al.
In: Nano Letters, Vol. 24, No. 5, 07.02.2024, p. 1553-1562.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

TY - JOUR

T1 - Steering the Selectivity of Carbon Dioxide Electroreduction from Single-Carbon to Multicarbon Products on Metal−Organic Frameworks via Facet Engineering

AU - Lu, Pengyi

AU - Lv, Jia

AU - Chen, Yu

AU - Ma, Yangbo

AU - Wang, Yunhao

AU - Lyu, Weichao

AU - Yu, Jinli

AU - Zhou, Jingwen

AU - Yin, Jinwen

AU - Xiong, Yuecheng

AU - Wang, Guozhi

AU - Ling, Chongyi

AU - Xi, Shibo

AU - Zhang, Daliang

AU - Fan, Zhanxi

PY - 2024/2/7

Y1 - 2024/2/7

N2 - Although metal−organic frameworks (MOFs) have attracted more attention for the electrocatalytic CO2 reduction reaction (CO2RR), obtaining multicarbon products with a high Faradaic efficiency (FE) remains challenging, especially under neutral conditions. Here, we report the controlled synthesis of stable Cu(I) 5-mercapto-1-methyltetrazole framework (Cu-MMT) nanostructures with different facets by rationally modulating the reaction solvents. Significantly, Cu-MMT nanostructures with (001) facets are acquired using isopropanol as a solvent, which favor multicarbon production with an FE of 73.75% and a multicarbon:single-carbon ratio of 3.93 for CO2RR in a neutral electrolyte. In sharp contrast, Cu-MMT nanostructures with (100) facets are obtained utilizing water, promoting single-carbon generation with an FE of 63.98% and a multicarbon: single-carbon ratio of only 0.18. Furthermore, this method can be extended to other Cu-MMT nanostructures with different facets in tuning the CO2 reduction selectivity. This work opens up new opportunities for the highly selective and efficient CO2 electroreduction to multicarbon products on MOFs via facet engineering. © 2024 American Chemical Society.

AB - Although metal−organic frameworks (MOFs) have attracted more attention for the electrocatalytic CO2 reduction reaction (CO2RR), obtaining multicarbon products with a high Faradaic efficiency (FE) remains challenging, especially under neutral conditions. Here, we report the controlled synthesis of stable Cu(I) 5-mercapto-1-methyltetrazole framework (Cu-MMT) nanostructures with different facets by rationally modulating the reaction solvents. Significantly, Cu-MMT nanostructures with (001) facets are acquired using isopropanol as a solvent, which favor multicarbon production with an FE of 73.75% and a multicarbon:single-carbon ratio of 3.93 for CO2RR in a neutral electrolyte. In sharp contrast, Cu-MMT nanostructures with (100) facets are obtained utilizing water, promoting single-carbon generation with an FE of 63.98% and a multicarbon: single-carbon ratio of only 0.18. Furthermore, this method can be extended to other Cu-MMT nanostructures with different facets in tuning the CO2 reduction selectivity. This work opens up new opportunities for the highly selective and efficient CO2 electroreduction to multicarbon products on MOFs via facet engineering. © 2024 American Chemical Society.

KW - carbon dioxide reduction reaction

KW - electrocatalysis

KW - facet engineering

KW - metal−organic frameworks

KW - multicarbon products

UR - https://www.scopus.com/pages/publications/85184519189

UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-85184519189&origin=recordpage

U2 - 10.1021/acs.nanolett.3c04092

DO - 10.1021/acs.nanolett.3c04092

M3 - RGC 21 - Publication in refereed journal

C2 - 38266492

SN - 1530-6984

VL - 24

SP - 1553

EP - 1562

JO - Nano Letters

JF - Nano Letters

IS - 5

ER -

Steering the Selectivity of Carbon Dioxide Electroreduction from Single-Carbon to Multicarbon Products on Metal−Organic Frameworks via Facet Engineering

Abstract

Funding

UN SDGs

Research Keywords

Publisher's Copyright Statement

RGC Funding Information

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ECS: Controlled Synthesis of Unconventional Phase Copper-based Janus Nanostructures for Tandem Electrocatalytic Carbon Dioxide Reduction

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Steering the Selectivity of Carbon Dioxide Electroreduction from Single-Carbon to Multicarbon Products on Metal−Organic Frameworks via Facet Engineering

Abstract

Funding

UN SDGs

Research Keywords

Publisher's Copyright Statement

RGC Funding Information

Access Output

Other Access Options

Permanent Link

Other Files and Links

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Projects

ECS: Controlled Synthesis of Unconventional Phase Copper-based Janus Nanostructures for Tandem Electrocatalytic Carbon Dioxide Reduction

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