College of Chemistry, Chemical Engineering and Materials Science, Soochow University , Jiangsu 215123, China.
Research Institute of Industrial Catalysis, School of Chemistry & Molecular Engineering, East China University of Science & Technology , Shanghai 200237, China.
J Am Chem Soc. 2017 May 24;139(20):6827-6830. doi: 10.1021/jacs.7b03101. Epub 2017 May 15.
Carbon dioxide (CO) hydrogenation to ethanol (CHOH) is considered a promising way for CO conversion and utilization, whereas desirable conversion efficiency remains a challenge. Herein, highly active, selective and stable CO hydrogenation to CHOH was enabled by highly ordered Pd-Cu nanoparticles (NPs). By tuning the composition of the Pd-Cu NPs and catalyst supports, the efficiency of CO hydrogenation to CHOH was well optimized with PdCu NPs/P25 exhibiting high selectivity to CHOH of up to 92.0% and the highest turnover frequency of 359.0 h. Diffuse reflectance infrared Fourier transform spectroscopy results revealed the high CHOH production and selectivity of PdCu NPs/P25 can be ascribed to boosting *CO (adsorption CO) hydrogenation to *HCO, the rate-determining step for the CO hydrogenation to CHOH.
二氧化碳(CO)加氢合成乙醇(CHOH)被认为是一种很有前途的 CO 转化和利用方法,但所需的转化效率仍然是一个挑战。在此,通过高度有序的钯-铜纳米粒子(NPs)实现了对 CO 加氢合成 CHOH 的高活性、选择性和稳定性。通过调整 Pd-Cu NPs 的组成和催化剂载体,PdCu NPs/P25 对 CO 加氢合成 CHOH 的效率得到了很好的优化,其选择性高达 92.0%,最高转化频率为 359.0 h。漫反射红外傅里叶变换光谱结果表明,PdCu NPs/P25 具有高 CHOH 产率和选择性,可归因于促进CO(吸附 CO)加氢生成HCO,这是 CO 加氢合成 CHOH 的速率决定步骤。