Light-Assisted CO2 Cycloaddition over a Nanochannel Cadmium–Organic Framework Loaded with Silver Nanoparticles,ACS Applied Nano Materials

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Light-Assisted CO2 Cycloaddition over a Nanochannel Cadmium–Organic Framework Loaded with Silver Nanoparticles
ACS Applied Nano Materials ( IF 5.3 ) Pub Date : 2023-04-05 , DOI: 10.1021/acsanm.3c00499
Dan Wu ₁ , Xiangmei Lu ₁ , Yue Tang ₁ , Fei Gao ₁ , Guoping Yang ₁ , Yao-Yu Wang ₁

Affiliation

Compared to conventional thermal-driven fixation, the light-assisted CO₂ fixation into useful chemicals represents a viable strategy for environmental restoratio n and energy sustainability. Hence, in this work, the type of linker was tuned to control the structure and topology of metal–organic frameworks (MOFs), resulting in a diversity of pore networks ranging from two-dimensional (2D) microporous channels (NWU-Cd1, 2) to three-dimensional (3D) nanochannels (NWU-Cd3). Among them, NWU-Cd3 can be employed as a reducing agent to convert Ag(I) ions to Ag(0) to generate Ag/NWU-Cd3 composite materials in situ due to its large pore size, high CO₂ adsorption capacity, and redox activity. Ag/NWU-Cd3 can expand the absorption spectrum to the visible area, and it exhibits excellent photocatalytic activity with the yield of styrene carbonate up to 94.3% at light irradiation and room temperature, which is 5.2 times of that under dark conditions. Notably, each Ag NP of the MOF network functions concurrently as a photosensitizer (harvesting light and producing electrons) and a cocatalyst (serving as the Lewis acid). The plasmonic hot electrons can gather on the Ag NP surface under light irradiation and rapidly transfer to NWU-Cd3 to interact with CO₂, resulting in activated CO₂*. Simultaneously, the presence of Ag NPs provides an action site for epoxides and accelerates the ring-opening process, and thus, Ag/NWU-Cd3 displays high catalytic reactivity for CO₂ cycloaddition under mild circumstances (25 °C, 1 atm). This research clarifies the conjunction of light and Ag NPs in accelerating CO₂ conversion and offers a substitutable method to further devise effective heterogeneous catalysts for light-induced CO₂ cycloaddition.

中文翻译：

载有银纳米颗粒的纳米通道镉-有机骨架上的光辅助 CO2 环加成

与传统的热驱动固定相比，光辅助 CO ₂固定成有用的化学品代表了环境恢复和能源可持续性的可行策略。因此，在这项工作中，连接器的类型被调整以控制金属有机骨架 (MOF) 的结构和拓扑结构，从而产生从二维 (2D) 微孔通道 (NWU-Cd1, 2) 到孔隙网络的多样性) 到三维 (3D) 纳米通道 ( NWU-Cd3 )。其中，NWU-Cd3孔径大、CO ₂含量高，可作为还原剂将Ag(I)离子转化为Ag(0)，原位生成Ag/ NWU-Cd3复合材料。吸附容量和氧化还原活性。Ag/ NWU-Cd3可将吸收光谱扩展至可见光区，表现出优异的光催化活性，光照和室温条件下碳酸苯乙烯收率高达94.3%，是黑暗条件下的5.2倍。值得注意的是，MOF 网络中的每个 Ag NP 同时充当光敏剂（收集光并产生电子）和助催化剂（充当路易斯酸）。等离子体热电子在光照射下可以聚集在 Ag NP 表面并迅速转移到NWU-Cd3与 CO ₂相互作用，从而产生活化的 CO ₂*。同时，Ag NPs 的存在为环氧化物提供了一个作用位点并加速了开环过程，因此，Ag/ NWU-Cd3在温和的环境（25 °C，1 atm）下对 CO ₂环加成表现出高催化反应性。_{该研究阐明了光和 Ag NPs 在加速 CO 2}转化中的结合，并提供了一种可替代的方法来进一步设计用于光诱导 CO ₂环加成的有效非均相催化剂。

更新日期：2023-04-05

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