Selective CO2-to-Formate Conversion Driven by Visible Light over a Precious-Metal-Free Nonporous Coordination Polymer,ACS Catalysis

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Selective CO2-to-Formate Conversion Driven by Visible Light over a Precious-Metal-Free Nonporous Coordination Polymer
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-08-05 , DOI: 10.1021/acscatal.2c02177
Yoshinobu Kamakura _{1,

2} , Shuhei Yasuda ₃ , Naoki Hosokawa ₁ , Shunta Nishioka ₁ , Sawa Hongo ₄ , Toshiyuki Yokoi ₃ , Daisuke Tanaka ₄ , Kazuhiko Maeda ₁

Affiliation

Metal–organic frameworks (MOFs) and coordination polymers (CPs) are potential candidates for high-performance photocatalysts because of their high tunability of electronic and structural properties. For example, MOFs and CPs having a high specific surface area (∼1000 m² g^–1) have been applied as visible-light-driven photocatalysts for CO₂ reduction and water splitting. Herein, we show a unique CP possessing a metal–sulfur bond with Pb²⁺, an earth-abundant metal ion. Different from ordinary high-surface-area MOFs and CPs, this CP is nonporous and has just 0.7 m² g^–1 surface area. Nevertheless, owing to its capability of absorbing visible light up to ∼500 nm, it efficiently photocatalyzes CO₂ reduction to formate (HCOO^–) under visible-light irradiation with >99% selectivity and an apparent quantum yield of 2.6% at 400 nm, even without postmodification treatment such as cocatalyst loading. These values are the highest yet reported for a precious-metal-free single-component photocatalyst for the visible-light-driven reduction of CO₂ to HCOO^–. This work may thus shed light on the great potential of nonporous CPs as building units of photocatalytic CO₂ conversion systems.

中文翻译：

在无贵金属无孔配位聚合物上由可见光驱动的选择性 CO2 到甲酸盐的转化

金属有机框架（MOFs）和配位聚合物（CPs）是高性能光催化剂的潜在候选者，因为它们具有高度的电子和结构特性可调性。例如，具有高比表面积（~1000 m ² g ^-1）的 MOFs 和 CPs 已被用作可见光驱动的 CO ₂还原和水分解光催化剂。在此，我们展示了一种独特的 CP ，它与富含地球的金属离子Pb ²⁺具有金属-硫键。与普通的高表面积 MOF 和 CP 不同，这种 CP 是无孔的，只有 0.7 m ² g ^–1表面积。然而，由于其吸收高达~500 nm的可见光的能力，它在可见光照射下有效地光催化CO ₂还原为甲酸盐（HCOO ^-），选择性> 99%，在400 nm处的表观量子产率为2.6%，即使没有后改性处理，如助催化剂负载。_{对于可见光驱动的 CO 2}还原为 HCOO^的无贵金属单组分光催化剂，这些值是迄今为止报道的最高值。因此，这项工作可能会揭示无孔 CP 作为光催化 CO ₂转化系统的构建单元的巨大潜力。

更新日期：2022-08-05

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