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Ir-CoO Active Centers Supported on Porous Al2O3 Nanosheets as Efficient and Durable Photo-Thermal Catalysts for CO2 Conversion
Advanced Science ( IF 14.3 ) Pub Date : 2023-03-17 , DOI: 10.1002/advs.202300122
Yunxiang Tang 1 , Tingting Zhao 1 , Hecheng Han 2 , Zhengyi Yang 1 , Jiurong Liu 1 , Xiaodong Wen 3, 4 , Fenglong Wang 1, 5
Advanced Science ( IF 14.3 ) Pub Date : 2023-03-17 , DOI: 10.1002/advs.202300122
Yunxiang Tang 1 , Tingting Zhao 1 , Hecheng Han 2 , Zhengyi Yang 1 , Jiurong Liu 1 , Xiaodong Wen 3, 4 , Fenglong Wang 1, 5
Affiliation
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Photo-thermal catalytic CO2 hydrogenation is currently extensively studied as one of the most promising approaches for the conversion of CO2 into value-added chemicals under mild conditions; however, achieving desirable conversion efficiency and target product selectivity remains challenging. Herein, the fabrication of Ir-CoO/Al2O3 catalysts derived from Ir/CoAl LDH composites is reported for photo-thermal CO2 methanation, which consist of Ir-CoO ensembles as active centers that are evenly anchored on amorphous Al2O3 nanosheets. A CH4 production rate of 128.9 mmol gcat⁻1 h⁻1 is achieved at 250 °C under ambient pressure and visible light irradiation, outperforming most reported metal-based catalysts. Mechanism studies based on density functional theory (DFT) calculations and numerical simulations reveal that the CoO nanoparticles function as photocatalysts to donate electrons for Ir nanoparticles and meanwhile act as “nanoheaters” to effectively elevate the local temperature around Ir active sites, thus promoting the adsorption, activation, and conversion of reactant molecules. In situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) demonstrates that illumination also efficiently boosts the conversion of formate intermediates. The mechanism of dual functions of photothermal semiconductors as photocatalysts for electron donation and as nano-heaters for local temperature enhancement provides new insight in the exploration for efficient photo-thermal catalysts.
中文翻译：
Ir-CoO 活性中心负载在多孔 Al2O3 纳米片上作为高效耐用的 CO2 转化光热催化剂
光热催化 CO 2加氢目前作为在温和条件下将 CO 2转化为增值化学品的最有前途的方法之一得到广泛研究；然而，实现理想的转化效率和目标产物选择性仍然具有挑战性。在此，报道了由 Ir/CoAl LDH 复合材料制备的 Ir-CoO/Al 2 O 3催化剂用于光热 CO 2甲烷化，该催化剂由均匀锚定在非晶 Al 2 O上的 Ir-CoO 系综作为活性中心组成3纳米片。CH 4产率为 128.9 mmol g cat⁻ 1 h⁻ 1在环境压力和可见光照射下，在 250 °C 下实现，优于大多数报道的金属基催化剂。基于密度泛函理论 (DFT) 计算和数值模拟的机理研究表明，Co3O 纳米粒子作为光催化剂为 Ir 纳米粒子提供电子，同时作为“纳米加热器”有效地提高 Ir 活性位点周围的局部温度，从而促进吸附、活化和反应物分子的转化。原位漫反射红外傅里叶变换光谱（原位 DRIFTS）表明，照明也能有效促进甲酸盐中间体的转化。
更新日期：2023-03-17
中文翻译：
Ir-CoO 活性中心负载在多孔 Al2O3 纳米片上作为高效耐用的 CO2 转化光热催化剂
光热催化 CO 2加氢目前作为在温和条件下将 CO 2转化为增值化学品的最有前途的方法之一得到广泛研究；然而，实现理想的转化效率和目标产物选择性仍然具有挑战性。在此，报道了由 Ir/CoAl LDH 复合材料制备的 Ir-CoO/Al 2 O 3催化剂用于光热 CO 2甲烷化，该催化剂由均匀锚定在非晶 Al 2 O上的 Ir-CoO 系综作为活性中心组成3纳米片。CH 4产率为 128.9 mmol g cat⁻ 1 h⁻ 1在环境压力和可见光照射下，在 250 °C 下实现，优于大多数报道的金属基催化剂。基于密度泛函理论 (DFT) 计算和数值模拟的机理研究表明，Co3O 纳米粒子作为光催化剂为 Ir 纳米粒子提供电子，同时作为“纳米加热器”有效地提高 Ir 活性位点周围的局部温度，从而促进吸附、活化和反应物分子的转化。原位漫反射红外傅里叶变换光谱（原位 DRIFTS）表明，照明也能有效促进甲酸盐中间体的转化。
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