Tuning Internal Strain in Metal-Organic Frameworks via Vapor Phase Infiltration for CO2 Reduction

被引：42

作者：

Yang, Fan ^{[1
]}

Hu, Wenhui ^{[2
]}

Yang, Chongqing ^{[3
]}

Patrick, Margaret ^{[1
]}

Cooksy, Andrew L. ^{[1
]}

Zhang, Jian ^{[3
]}

Aguiar, Jeffery A. ^{[4
]}

Fang, Chengcheng ^{[5
]}

Zhou, Yinghua ^{[1
,6
]}

Meng, Ying Shirley ^{[5
]}

Huang, Jier ^{[2
]}

Gu, Jing ^{[1
]}

机构：

[1] San Diego State Univ, Dept Chem & Biochem, 5500 Campanile Dr, San Diego, CA 92182 USA

[2] Marquette Univ, Dept Chem, Milwaukee, WI 53201 USA

[3] Lawrence Berkeley Natl Lab, Mol Foundry, Berkeley, CA 94720 USA

[4] Idaho Natl Lab, Nucl Mat Dept, 2525 Fremt Ave, Idaho Falls, ID 83415 USA

[5] Univ Calif San Diego, Mat Sci & Engn Program, La Jolla, CA 92093 USA

[6] Anhui Normal Univ, Coll Chem & Mat Sci, Anhui Lab Mol Based Mat, Key Lab Funct Mol Solids,Minist Educ, Wuhu 241000, Peoples R China

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2020年 / 59卷 / 11期

基金：

美国国家科学基金会; 中国国家自然科学基金;

关键词：

CO2; reduction; internal strain; metal-organic frameworks; vapor-phase infiltration; ATOMIC LAYER DEPOSITION; ELECTROCATALYTIC REDUCTION; CARBON-DIOXIDE; THIN-FILMS; ELECTROREDUCTION; NANOCOMPOSITE; PHOTOANODES; PORPHYRINS; CATALYSTS;

D O I：

10.1002/anie.202000022

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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 200-300 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.

引用

页码：4572 / 4580

页数：9

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