Tuning Internal Strain in Metal–Organic Frameworks via Vapor Phase Infiltration for CO2 Reduction
Abstract
A gas-phase approach to form Zn coordination sites on metal-organic frameworks (MOFs) by vapor-phase infiltration (VPI) was developed. Compared to Zn sites synthesized by the solution-phase method, VPI samples revealed approximately 2.8 % internal strain. Faradaic efficiency towards conversion of CO2 to CO was enhanced by up to a factor of four, and the initial potential was positively shifted by 200-30 mV. Using element-specific X-ray absorption spectroscopy, the local coordination environment of the Zn center was determined to have square-pyramidal geometry with four Zn-N bonds in the equatorial plane and one Zn-OH2 bond in the axial plane. The fine-tuned internal strain was further supported by monitoring changes in XRD and UV/Visible absorption spectra across a range of infiltration cycles. The ability to use internal strain to increase catalytic activity of MOFs suggests that applying this strategy will enhance intrinsic catalytic capabilities of a variety of porous materials.
- Authors:
-
[1]
- San Diego State Univ., CA (United States). Dept. of Chemistry and Biochemistry
- Marquette Univ., Milwaukee, WI (United States). Dept. of Chemistry
- The Molecular FoundryLawrence Berkeley National Laboratory Berkeley CA 94720 USA
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
- Idaho National Lab. (INL), Idaho Falls, ID (United States). Nuclear Materials Dept.
- Univ. of California, San Diego, CA (United States). Materials Science and Engineering Program
- San Diego State Univ., CA (United States). Dept. of Chemistry and Biochemistry; Anhui Normal Univ., Wuhu (China). The Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Laboratory of Molecule-Based Materials, College of Chemistry and Materials Science
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1779238
- Alternate Identifier(s):
- OSTI ID: 1595851
- Grant/Contract Number:
- AC02-05CH11231; DMR-1654140; CBET-1704992
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 59; Journal Issue: 11; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; CO2 reduction; internal strain; metal-organic frameworks; vapor-phase infiltration
Citation Formats
Yang, Fan, Hu, Wenhui, Yang, Chongqing, Patrick, Margaret, Cooksy, Andrew L., Zhang, Jian, Aguiar, Jeffery A., Fang, Chengcheng, Zhou, Yinghua, Meng, Ying Shirley, Huang, Jier, and Gu, Jing. Tuning Internal Strain in Metal–Organic Frameworks via Vapor Phase Infiltration for CO2 Reduction. United States: N. p., 2020.
Web. doi:10.1002/anie.202000022.
Yang, Fan, Hu, Wenhui, Yang, Chongqing, Patrick, Margaret, Cooksy, Andrew L., Zhang, Jian, Aguiar, Jeffery A., Fang, Chengcheng, Zhou, Yinghua, Meng, Ying Shirley, Huang, Jier, & Gu, Jing. Tuning Internal Strain in Metal–Organic Frameworks via Vapor Phase Infiltration for CO2 Reduction. United States. https://doi.org/10.1002/anie.202000022
Yang, Fan, Hu, Wenhui, Yang, Chongqing, Patrick, Margaret, Cooksy, Andrew L., Zhang, Jian, Aguiar, Jeffery A., Fang, Chengcheng, Zhou, Yinghua, Meng, Ying Shirley, Huang, Jier, and Gu, Jing. Wed .
"Tuning Internal Strain in Metal–Organic Frameworks via Vapor Phase Infiltration for CO2 Reduction". United States. https://doi.org/10.1002/anie.202000022. https://www.osti.gov/servlets/purl/1779238.
@article{osti_1779238,
title = {Tuning Internal Strain in Metal–Organic Frameworks via Vapor Phase Infiltration for CO2 Reduction},
author = {Yang, Fan and Hu, Wenhui and Yang, Chongqing and Patrick, Margaret and Cooksy, Andrew L. and Zhang, Jian and Aguiar, Jeffery A. and Fang, Chengcheng and Zhou, Yinghua and Meng, Ying Shirley and Huang, Jier and Gu, Jing},
abstractNote = {A gas-phase approach to form Zn coordination sites on metal-organic frameworks (MOFs) by vapor-phase infiltration (VPI) was developed. Compared to Zn sites synthesized by the solution-phase method, VPI samples revealed approximately 2.8 % internal strain. Faradaic efficiency towards conversion of CO2 to CO was enhanced by up to a factor of four, and the initial potential was positively shifted by 200-30 mV. Using element-specific X-ray absorption spectroscopy, the local coordination environment of the Zn center was determined to have square-pyramidal geometry with four Zn-N bonds in the equatorial plane and one Zn-OH2 bond in the axial plane. The fine-tuned internal strain was further supported by monitoring changes in XRD and UV/Visible absorption spectra across a range of infiltration cycles. The ability to use internal strain to increase catalytic activity of MOFs suggests that applying this strategy will enhance intrinsic catalytic capabilities of a variety of porous materials.},
doi = {10.1002/anie.202000022},
journal = {Angewandte Chemie (International Edition)},
number = 11,
volume = 59,
place = {United States},
year = {2020},
month = {1}
}
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