Selective photocatalytic production of CH4 using Zn-based polyoxometalate as a nonconventional CO2 reduction catalyst

被引：18

作者：

Kim, Nayeong ^{[1
,2
]}

Nam, Jung Seung ^{[3
,4
]}

Jo, Jinhyeong ^{[1
]}

Seong, Junmo ^{[3
]}

Kim, Hyunwoo ^{[1
,2
]}

Kwon, Youngkook ^{[2
,5
]}

Lah, Myoung Soo ^{[3
]}

Lee, Jun Hee ^{[1
]}

Kwon, Tae-Hyuk ^{[3
,4
]}

Ryu, Jungki ^{[1
,2
]}

机构：

[1] Ulsan Natl Inst Sci & Technol UNIST, Sch Energy & Chem Engn, Dept Energy Engn, 50 UNIST Gil, Ulsan 44919, South Korea

[2] Ulsan Natl Inst Sci & Technol UNIST, Emergent Hydrogen Technol R&D Ctr, 50 UNIST Gil, Ulsan 44919, South Korea

[3] Ulsan Natl Inst Sci & Technol UNIST, Sch Nat Sci, Dept Chem, 50 UNIST Gil, Ulsan 44919, South Korea

[4] Ulsan Natl Inst Sci & Technol UNIST, Sch Nat Sci, Ctr Wave Energy Mat, 50 UNIST Gil, Ulsan 44919, South Korea

[5] Ulsan Natl Inst Sci & Technol UNIST, Sch Energy & Chem Engn, 50 UNIST Gil, Ulsan 44919, South Korea

来源：

NANOSCALE HORIZONS | 2021年 / 6卷 / 05期

基金：

新加坡国家研究基金会;

关键词：

NOBLE-METAL-FREE; CARBON-DIOXIDE; ELECTROCHEMICAL REDUCTION; ACTIVE-SITES; EFFICIENT; CONVERSION; METHANE;

D O I：

10.1039/d0nh00657b

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Efficient and selective production of CH4 through the CO2 reduction reaction (CO2RR) is a challenging task due to the high amount of energy consumption and various reaction pathways. Here, we report the synthesis of Zn-based polyoxometalate (ZnPOM) and its application in the photocatalytic CO2RR. Unlike conventional Zn-based catalysts that produce CO, ZnPOM can selectively catalyze the production of CH4 in the presence of an Ir-based photosensitizer (TIr3) through the photocatalytic CO2RR. Photophysical and computation analyses suggest that selective photocatalytic production of CH4 using ZnPOM and TIr3 can be attributed to (1) the exceptionally fast transfer of photogenerated electrons from TIr3 to ZnPOM through the strong molecular interactions between them and (2) effective transfer of electrons from ZnPOM to *CO intermediates due to significant hybridization of their molecular orbitals. This study provides insights into the design of novel CO2RR catalysts for CH4 production beyond the limitations in conventional studies that focus on Cu-based materials.

引用

页码：379 / 385

页数：7

共 45 条

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