MOF-Derived Robust and Synergetic Acid Sites Inducing C-N Bond Disruption for Energy-Efficient CO2Desorption

Lei Xing; Meng Li; Mingyue Li; Teng Xu; Yuchen Li; Tieyue Qi; Huanxin Li; Zhigang Hu; Guang Ping Hao; Shihan Zhang; Tony David James; Boyang Mao; Lidong Wang

doi:10.1021/acs.est.2c06842

MOF-Derived Robust and Synergetic Acid Sites Inducing C-N Bond Disruption for Energy-Efficient CO₂Desorption

Lei Xing
, Meng Li
, Mingyue Li
, Teng Xu
, Yuchen Li
, Tieyue Qi
, Huanxin Li
, Zhigang Hu
, Guang Ping Hao
, Shihan Zhang
, Tony David James
, Boyang Mao
, Lidong Wang

North China Electric Power University
Tsinghua University
MOE
University of Cambridge
Dalian University of Technology
Zhejiang University of Technology

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

65 Citations (SciVal)

193 Downloads (Pure)

Abstract

Amine-based scrubbing technique is recognized as a promising method of capturing CO2 to alleviate climate change. However, the less stability and poor acidity of solid acid catalysts (SACs) limit their potential to further improve amine regeneration activity and reduce the energy penalty. To address these challenges, here, we introduce two-dimensional (2D) cobalt-nitrogen-doped carbon nanoflakes (Co-N-C NSs) driven by a layered metal-organic framework that work as SACs. The designed 2D Co-N-C SACs can exhibit promising stability, superhydrophilic surface, and acidity. Such 2D structure also contains well-confined Co-N4 Lewis acid sites and -OH Brønsted acid sites to have a synergetic effect on C-N bond disruption and significantly increase CO2 desorption rate by 281% and reduce the reaction temperatures to 88 °C, minimizing water evaporation by 20.3% and subsequent regeneration energy penalty by 71.7% compared to the noncatalysis.

Original language	English
Pages (from-to)	17936-17945
Number of pages	10
Journal	Environmental Science and Technology
Volume	56
Issue number	24
DOIs	https://doi.org/10.1021/acs.est.2c06842
Publication status	Published - 20 Dec 2022

Bibliographical note

Funding Information:
This research was supported by the National Natural Science Foundation of China (nos. 21706061, 21876157, 22176057, and 22276051), China Postdoctoral Science Foundation (2022TQ0175), and the Central Government Guided Local Science and Technology Development Fund (nos. 2021ZY1022 and XM2112344).

Funding

This research was supported by the National Natural Science Foundation of China (nos. 21706061, 21876157, 22176057, and 22276051), China Postdoctoral Science Foundation (2022TQ0175), and the Central Government Guided Local Science and Technology Development Fund (nos. 2021ZY1022 and XM2112344).

UN SDGs

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

SDG 7 Affordable and Clean Energy
SDG 13 Climate Action

Keywords

2D nanoflakes
COcapture
energy efficiency
MEA regeneration
solid acid catalyst

ASJC Scopus subject areas

General Chemistry
Environmental Chemistry

Access to Document

10.1021/acs.est.2c06842

MOF CO2Accepted author manuscript, 1.08 MB

Cite this

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title = "MOF-Derived Robust and Synergetic Acid Sites Inducing C-N Bond Disruption for Energy-Efficient CO2Desorption",

abstract = "Amine-based scrubbing technique is recognized as a promising method of capturing CO2 to alleviate climate change. However, the less stability and poor acidity of solid acid catalysts (SACs) limit their potential to further improve amine regeneration activity and reduce the energy penalty. To address these challenges, here, we introduce two-dimensional (2D) cobalt-nitrogen-doped carbon nanoflakes (Co-N-C NSs) driven by a layered metal-organic framework that work as SACs. The designed 2D Co-N-C SACs can exhibit promising stability, superhydrophilic surface, and acidity. Such 2D structure also contains well-confined Co-N4 Lewis acid sites and -OH Br{\o}nsted acid sites to have a synergetic effect on C-N bond disruption and significantly increase CO2 desorption rate by 281\% and reduce the reaction temperatures to 88 °C, minimizing water evaporation by 20.3\% and subsequent regeneration energy penalty by 71.7\% compared to the noncatalysis.",

keywords = "2D nanoflakes, COcapture, energy efficiency, MEA regeneration, solid acid catalyst",

author = "Lei Xing and Meng Li and Mingyue Li and Teng Xu and Yuchen Li and Tieyue Qi and Huanxin Li and Zhigang Hu and Hao, \{Guang Ping\} and Shihan Zhang and James, \{Tony David\} and Boyang Mao and Lidong Wang",

note = "Funding Information: This research was supported by the National Natural Science Foundation of China (nos. 21706061, 21876157, 22176057, and 22276051), China Postdoctoral Science Foundation (2022TQ0175), and the Central Government Guided Local Science and Technology Development Fund (nos. 2021ZY1022 and XM2112344). ",

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month = dec,

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doi = "10.1021/acs.est.2c06842",

language = "English",

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journal = "Environmental Science and Technology",

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TY - JOUR

T1 - MOF-Derived Robust and Synergetic Acid Sites Inducing C-N Bond Disruption for Energy-Efficient CO2Desorption

AU - Xing, Lei

AU - Li, Meng

AU - Li, Mingyue

AU - Xu, Teng

AU - Li, Yuchen

AU - Qi, Tieyue

AU - Li, Huanxin

AU - Hu, Zhigang

AU - Hao, Guang Ping

AU - Zhang, Shihan

AU - James, Tony David

AU - Mao, Boyang

AU - Wang, Lidong

N1 - Funding Information: This research was supported by the National Natural Science Foundation of China (nos. 21706061, 21876157, 22176057, and 22276051), China Postdoctoral Science Foundation (2022TQ0175), and the Central Government Guided Local Science and Technology Development Fund (nos. 2021ZY1022 and XM2112344).

PY - 2022/12/20

Y1 - 2022/12/20

N2 - Amine-based scrubbing technique is recognized as a promising method of capturing CO2 to alleviate climate change. However, the less stability and poor acidity of solid acid catalysts (SACs) limit their potential to further improve amine regeneration activity and reduce the energy penalty. To address these challenges, here, we introduce two-dimensional (2D) cobalt-nitrogen-doped carbon nanoflakes (Co-N-C NSs) driven by a layered metal-organic framework that work as SACs. The designed 2D Co-N-C SACs can exhibit promising stability, superhydrophilic surface, and acidity. Such 2D structure also contains well-confined Co-N4 Lewis acid sites and -OH Brønsted acid sites to have a synergetic effect on C-N bond disruption and significantly increase CO2 desorption rate by 281% and reduce the reaction temperatures to 88 °C, minimizing water evaporation by 20.3% and subsequent regeneration energy penalty by 71.7% compared to the noncatalysis.

AB - Amine-based scrubbing technique is recognized as a promising method of capturing CO2 to alleviate climate change. However, the less stability and poor acidity of solid acid catalysts (SACs) limit their potential to further improve amine regeneration activity and reduce the energy penalty. To address these challenges, here, we introduce two-dimensional (2D) cobalt-nitrogen-doped carbon nanoflakes (Co-N-C NSs) driven by a layered metal-organic framework that work as SACs. The designed 2D Co-N-C SACs can exhibit promising stability, superhydrophilic surface, and acidity. Such 2D structure also contains well-confined Co-N4 Lewis acid sites and -OH Brønsted acid sites to have a synergetic effect on C-N bond disruption and significantly increase CO2 desorption rate by 281% and reduce the reaction temperatures to 88 °C, minimizing water evaporation by 20.3% and subsequent regeneration energy penalty by 71.7% compared to the noncatalysis.

KW - 2D nanoflakes

KW - COcapture

KW - energy efficiency

KW - MEA regeneration

KW - solid acid catalyst

UR - https://www.scopus.com/pages/publications/85143857808

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DO - 10.1021/acs.est.2c06842

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