TiO2/Au 纳米复合材料电化学还原二氧化碳,ACS Applied Materials & Interfaces

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TiO2/Au 纳米复合材料电化学还原二氧化碳
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2022-11-08 , DOI: 10.1021/acsami.2c14368
M Nur Hossain ₁ , Rachelle M Choueiri ₁ , Sharon Abner ₁ , Leanne D Chen ₁ , Aicheng Chen ₁

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在此，我们报告了通过定制的电流置换反应 (GRR) 轻松合成由 TiO ₂和 Au 纳米颗粒 (NPs) 组成的纳米复合材料。使用各种电化学方法在水溶液中研究了合成的 TiO ₂ /Au 纳米复合材料对 CO _{2还原的电催化活性。}我们的结果表明，与多晶 Au 相比，通过 GRR 工艺形成的 TiO ₂ /Au 纳米复合材料表现出改善的 CO ₂还原催化活性，同时产生比典型的 CO 形成更多的碳氢化合物分子。GC 分析和 NMR 光谱显示 CO 和 CH ₄是气体产物，而 HCOO^–、CH ₃ COO ^–、CH ₃ OH 和CH ₃ CH ₂ OH 是不同阴极电位下CO ₂还原的液体产物。使用密度泛函理论 (DFT) 计算进一步研究了这一显着变化，表明与 Au 相比，TiO ₂ /Au 纳米复合材料可以增加形成的^· CO 中间体的结合能并降低自由能，从而有利于下游生成多碳产品。_二氧化钛/Au纳米复合材料具有高催化活性和优异的稳定性，且易于制备，表明所开发的催化剂在电化学还原CO ₂为高附加值产品方面具有潜在的应用前景。

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Electrochemical Reduction of Carbon Dioxide at TiO2/Au Nanocomposites

Herein, we report on the facile synthesis of nanocomposite consisting of TiO₂ and Au nanoparticles (NPs) via a tailored galvanic replacement reaction (GRR). The electrocatalytic activity of the synthesized TiO₂/Au nanocomposites for CO₂ reduction was investigated in an aqueous solution using various electrochemical methods. Our results demonstrated that the TiO₂/Au nanocomposites formed through the GRR process exhibited improved catalytic activities for CO₂ reduction, while generating more hydrocarbon molecules than the typical formation of CO in contrast to polycrystalline Au. GC analysis and NMR spectroscopy revealed that CO and CH₄ were the gas products, whereas HCOO^–, CH₃COO^–, CH₃OH, and CH₃CH₂OH were the liquid products from the CO₂ reduction at different cathodic potentials. This remarkable change was further studied using the density functional theory (DFT) calculations, showing that the TiO₂/Au nanocomposites may increase the binding energy of the formed ^·CO intermediate and reduce the free energy compared to Au, thus favoring the downstream generation of multicarbon products. The TiO₂/Au nanocomposites have high catalytic activity and excellent stability and are easy to fabricate, indicating that the developed catalyst has potential application in the electrochemical reduction of CO₂ to value-added products.

更新日期：2022-11-08

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