轻松室温合成无贵金属配位聚合物光催化剂以改善可见光二氧化碳减排,Solar RRL

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轻松室温合成无贵金属配位聚合物光催化剂以改善可见光二氧化碳减排
Solar RRL ( IF 6.0 ) Pub Date : 2023-11-09 , DOI: 10.1002/solr.202300710
Chomponoot Suppaso ₁ , Yoshinobu Kamakura ₁ , Misaki Ueno ₂ , Sawa Hongo ₂ , Ryohei Akiyoshi ₂ , Fumitaka Ishiwari _{3,

4,

5} , Akinori Saeki _{3,

4} , Daisuke Tanaka ₂ , Kazuhiko Maeda _{1,

6}

Affiliation

Pb-S基配位聚合物（CP），命名为KGF-9，[Pb(tadt)] _n（tadt = 1,3,4-噻二唑-2,5-二硫醇盐），可以选择性地将CO ₂转化为HCOO ^- (>99%) 在可见光下，400 nm 处的表观量子产率 (AQY) 为 2.6%，无需助催化剂。然而，KGF-9本质上是一种无孔CP，其较小的比表面积（<1 m ² g ^-1）可能会阻碍其作为光催化剂的全部潜力的实现。在此，报道了使用乙酸铅（II）作为前体，通过固相反应和液相反应（LPR）在室温下简便的合成路线。乙酸铅(II)的使用促进了H ₂ tadt配体的去质子化，从而导致更快的配位反应、减小的特征尺寸以及比表面积的急剧增加(≈10 m ² g ^-1 )。通过 60 分钟 LPR 制备的 KGF-9 发现甲酸盐产量较高的 AQY（400 nm 处为 5.9%）。LPR 样品光催化活性的提高归因于长寿命电荷载流子的存在，时间分辨微波电导率测量揭示了这一点。这项研究的结果为提高 CP 基光催化剂的活性提供了一种简单但有效的策略。

"点击查看英文标题和摘要"

Facile Room Temperature Synthesis of Precious-Metal-Free Coordination Polymer Photocatalyst for Improved Visible-Light CO2 Reduction

The Pb–S-based coordination polymer (CP), named KGF-9, [Pb(tadt)]_n (tadt = 1,3,4-thiadiazole-2,5-dithiolate), can selectively convert CO₂ into HCOO⁻ (>99%) under visible light, with an apparent quantum yield (AQY) of 2.6% at 400 nm, without a cocatalyst. However, KGF-9 is an intrinsically nonporous CP, and its small specific surface area (<1 m² g⁻¹) might hinder the realization of its full potential as a photocatalyst. Herein, facile synthetic routes at room temperature are reported through a solid-state reaction and a liquid-phase reaction (LPR) using lead(II) acetate as a precursor. The use of lead(II) acetate promotes the deprotonation of the H₂tadt ligand, resulting in a faster coordination reaction, a reduced feature size, and a drastic increase in specific surface area (≈10 m² g⁻¹). A higher AQY for formate production (5.9% at 400 nm) is found for KGF-9 prepared via a 60 min LPR. The improved photocatalytic activity of the LPR sample is attributed to the presence of long-lived charge carriers, which is revealed by time-resolved microwave conductivity measurements. The results of this study provide a simple but effective strategy toward increasing the activity of CP-based photocatalysts.

更新日期：2023-11-09

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