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研究报告

袁欢,刘欢,杨胜峰,陈子扬,叶代启,陈礼敏.水热溶剂对Cu/CeO₂-TiO₂催化CO₂加氢制甲醇反应性能的影响[J].环境科学学报,2022,42(12):353-365

Effects of hydrothermal solvents on the catalytic performance of Cu/CeO₂-TiO₂ catalysts for CO₂ hydrogenation to methanol

叶代启
华南理工大学环境与能源学院，广州 510006;挥发性有机物污染治理技术与装备国家工程实验室，广州 510006;广东省大气环境与污染控制重点实验室，广州 510006

陈礼敏
华南理工大学环境与能源学院，广州 510006;挥发性有机物污染治理技术与装备国家工程实验室，广州 510006;广东省大气环境与污染控制重点实验室，广州 510006

摘要：以高暴露（001）面锐钛矿TiO₂为载体，使用3种不同溶剂（甲醇、乙二醇和丙三醇）水热负载CeO₂，进而以CeO₂-TiO₂为载体采用硼氢化钠还原法负载Cu，合成Cu/CeO₂-TiO₂催化剂用于催化CO₂加氢制甲醇.XRD、SEM、BET、ICP-OES、XPS、H₂-TPR、EPR和CO₂-TPD等表征表明，以甲醇/水为混合溶剂合成的CeO₂-TiO₂（CT-M）载体中CeO₂粒径较小、Ce³⁺浓度较高，更有利于Cu的负载与分散，形成紧密接触的三相界面；其负载Cu的催化剂CCT-M经焙烧、还原后形成的CuCeTi三相界面相互作用更强，可产生更多的表面Ce³⁺、氧空位和体相Ti³⁺，表面Ce³⁺、氧空位和体相Ti³⁺等缺陷有利于CO₂的吸附活化，较小粒径的Cu则可加速氢解离，因此，CCT-M具有更多的CO₂加氢反应活性位点，表现出最优的CO₂加氢产甲醇活性.

Abstract：Cu/CeO₂-TiO₂ catalysts for CO₂ hydrogenation to methanol were synthesized by means of hydrothermal loading CeO₂ onto anatase TiO₂ with highly exposed（001）facets using three different solvents（methanol， ethylene glycol and glycerol）， following by loading Cu through NaBH₄ reduction method. XRD， SEM， BET， ICP-OES， XPS， H₂-TPR， EPR and CO₂-TPD characterizations indicate that CT-M using methanol/water as solvent is in favor of Cu loading and dispersion as a result of the smallest CeO₂particle diameter and the highest Ce³⁺ concentration， leading to the closely contact three-phase interface. After loading Cu， the interactions between Cu-CeO_x-TiO₂ three-phase interface over CCT-M catalyst are stronger during calcination and reduction process， producing more defects such as surface Ce³⁺， oxygen vacancies and bulk Ti³⁺， which are beneficial for the adsorption and activation of CO₂. In addition， Cu species with smaller particle size accelerate the hydrogen dissociation. Therefore， CCT-M catalyst has more active sites for CO₂ hydrogenation， exhibiting optimal CO₂ hydrogenation to methanol activity.

Key words：CO₂ hydrogenation methanol Cu/CeO₂-TiO₂ particle size charge transfer defect