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

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Selective photocatalytic production of CH4 using Zn-based polyoxometalate as a nonconventional CO2 reduction catalyst
Nanoscale Horizons ( IF 8.0 ) Pub Date : 2021-2-19 , DOI: 10.1039/d0nh00657b
Nayeong Kim _{1,

2,

3,

4,

5} , Jung Seung Nam _{3,

4,

5,

6,

7} , Jinhyeong Jo _{1,

2,

3,

4,

5} , Junmo Seong _{3,

4,

5,

6,

7} , Hyunwoo Kim _{1,

2,

3,

4,

5} , Youngkook Kwon _{3,

4,

5,

8,

9} , Myoung Soo Lah _{3,

4,

5,

6,

7} , Jun Hee Lee _{1,

2,

3,

4,

5} , Tae-Hyuk Kwon _{3,

4,

5,

6,

7} , Jungki Ryu _{1,

2,

3,

4,

5}

Affiliation

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.

中文翻译：

使用锌基多金属氧酸盐作为非常规的CO2还原催化剂选择性地光催化生产CH4

由于CO ₂还原反应（CO ₂ RR）的大量能量消耗和各种反应途径，有效和选择性地生产CH ₄是一项具有挑战性的任务。在这里，我们报告了锌基多金属氧酸盐（ZnPOM）的合成及其在光催化CO2RR中的应用。与产生CO的常规Zn基催化剂不同，ZnPOM可以在Ir基光敏剂（TIr3）的存在下通过光催化CO2RR选择性催化CH ₄的产生。光物理和计算分析表明，CH _4的选择性光催化生产使用ZnPOM和TIr3可以归因于（1）光生电子通过它们之间的强分子相互作用从TIr3到ZnPOM的异常快速转移，以及（2）由于其分子之间的显着杂交，电子从ZnPOM到* CO中间体的有效转移轨道。这项研究提供了对用于CH ₄生产的新型CO2RR催化剂的设计的见解，超越了常规研究（专注于铜基材料）的局限性。

更新日期：2021-03-15

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