[Ir(ppy) 2 (H2dcbpy)]和分子镍配合物在光催化CO2还原金属-有机框架中的功能集成

IF 3.9 3区 化学 Q2 CHEMISTRY, PHYSICAL
ChemCatChem Pub Date : 2025-07-27 DOI:10.1002/cctc.202500844
Osman Ali, Aruntima Das, Anupam Jana, Sinjini Mandal, Ashadul Adalder, Dr. Bholanath Maity, Dr. Asamanjoy Bhunia
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引用次数: 0

摘要

开发多功能光催化剂,有效地将CO₂转化为有价值的化学产品(如CO、CH4、HCOOH和CH3OH),对于实现可持续发展至关重要。为了解决这一挑战,我们报道了一种出色的多功能金属有机框架(MOF)光催化剂,称为UiO-67-Ni-Ir,它已经通过原位合成策略精心制作。这种前景看好的催化剂含有一个高效吸光铱单元,[Ir(ppy) 2 (H2dcbpy)](其中ppy = 2-苯基吡啶,H2dcbpy = 2,2 ' -联吡啶-4,4 ' -二羧酸),称为Ir- ps,与催化活性镍中心结合。Ir-PS装置对可见光的广泛吸收使其能够在可见光照射下进行高效的CO2还原反应。UiO-67-Ni-Ir光催化剂表现出优异的光催化性能,在6小时内产生5800µmol g - 1甲酸(HCOO - 1),选择性为96.5%。在相同的光催化过程中,超过51的周转数(TON)进一步支持了这种高甲酸收率,这比相应的均相体系高10倍。此外,该催化剂是完全多相和可回收的,使其成为可见光照射下CO2光催化转化为甲酸盐的有吸引力的候选者。此外,基于光物理和电化学研究以及密度泛函理论(DFT)提出了一个合理的机制,为潜在的催化过程提供了一个全面的理解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Functional Integration of [Ir(ppy)₂(H2dcbpy)] and a Molecular Nickel Complex into Metal-Organic Frameworks for Photocatalytic CO2 Reduction

Functional Integration of [Ir(ppy)₂(H2dcbpy)] and a Molecular Nickel Complex into Metal-Organic Frameworks for Photocatalytic CO2 Reduction

Functional Integration of [Ir(ppy)₂(H2dcbpy)] and a Molecular Nickel Complex into Metal-Organic Frameworks for Photocatalytic CO2 Reduction

Functional Integration of [Ir(ppy)₂(H2dcbpy)] and a Molecular Nickel Complex into Metal-Organic Frameworks for Photocatalytic CO2 Reduction

Developing multifunctional photocatalysts that efficiently convert CO₂ into valuable chemical products (e.g., CO, CH4, HCOOH, and CH3OH) is essential for achieving sustainable development. To address this challenge, we report a remarkable multifunctional metal-organic framework (MOF)-based photocatalyst, termed UiO-67-Ni-Ir, which has been elegantly crafted through an in situ synthesis strategy. This promising catalyst contains a highly efficient light-absorbing iridium unit, [Ir(ppy)₂(H2dcbpy)] (where ppy = 2-phenylpyridine, H2dcbpy = 2,2′-bipyridine-4,4′-dicarboxylic acid), referred to as Ir-PS, in conjunction with a catalytically active nickel center. The broad absorption of visible light of the Ir-PS unit empowers the efficient CO2 reduction reactions under visible light illumination. The photocatalyst UiO-67-Ni-Ir exhibits exceptional photocatalytic performance, producing 5800 µmol g−1 of formate (HCOO⁻) over a 6 h period with a remarkable selectivity of 96.5%. This high formate yield is further supported by a turnover number (TON) exceeding 51 during the same photocatalysis run, which is ten times higher than that of the corresponding homogeneous system. Moreover, this catalyst is completely heterogeneous and recyclable, making it an attractive candidate for the photocatalytic conversion of CO2 to formate under visible light irradiation. Furthermore, a plausible mechanism has been proposed based on the photophysical and electrochemical study along with density functional theory (DFT), which provides a comprehensive understanding of the underlying catalytic process.

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来源期刊
ChemCatChem
ChemCatChem 化学-物理化学
CiteScore
8.10
自引率
4.40%
发文量
511
审稿时长
1.3 months
期刊介绍: With an impact factor of 4.495 (2018), ChemCatChem is one of the premier journals in the field of catalysis. The journal provides primary research papers and critical secondary information on heterogeneous, homogeneous and bio- and nanocatalysis. The journal is well placed to strengthen cross-communication within between these communities. Its authors and readers come from academia, the chemical industry, and government laboratories across the world. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies, and is supported by the German Catalysis Society.
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