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Selective Ethanol Oxidation to Acetaldehyde on Nanostructured Zeolitic Imidazolate Framework-8-Wrapped ZnO Photothermocatalyst Thin Films
Solar RRL ( IF 6.0 ) Pub Date : 2020-10-23 , DOI: 10.1002/solr.202000423 Hao Wu 1, 2 , Tze Hao Tan 3 , Rugeng Liu 1 , Hsien‐Yi Hsu 1 , Yun Hau Ng 1, 2
Solar RRL ( IF 6.0 ) Pub Date : 2020-10-23 , DOI: 10.1002/solr.202000423 Hao Wu 1, 2 , Tze Hao Tan 3 , Rugeng Liu 1 , Hsien‐Yi Hsu 1 , Yun Hau Ng 1, 2
Affiliation
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Photothermocatalytic ethanol oxidation to acetaldehyde offers an alternative technology in synthesizing high-value-added chemicals. However, the practical application is hindered by the competition from overoxidation leading to complete mineralization. Herein, the 1D nanostructured ZnO@zeolitic imidazolate framework-8 (ZIF-8) composite is reported as an efficient photothermocatalyst, which shows improved conversion efficiency and high catalytic selectivity and durability compared with the parent ZnO nanorods, for continuous ethanol oxidation in a flow system. The ZnO@ZIF-8 composite achieves a high selectivity of 91.5% toward acetaldehyde production. The underlying mechanism is probed using electrochemical impedance spectroscopy, N2 adsorption–desorption isotherms, transient open-circuit potential, and steady-state and time-resolved photoluminescence spectroscopy. Collectively, the probings show that the improved performance originates from 1) facilitated charge separation; 2) lowered oxidation potential holes; 3) enlarged surface area; and 4) preferred reaction routes. This work provides a new perspective for the design of a hybrid photothermocatalyst for selective solar energy conversion into desirable chemicals.
中文翻译：
在纳米结构沸石咪唑酯骨架-8 包裹的 ZnO 光热催化剂薄膜上选择性乙醇氧化成乙醛
光热催化乙醇氧化为乙醛为合成高附加值化学品提供了一种替代技术。然而，过度氧化导致完全矿化的竞争阻碍了实际应用。在此，一维纳米结构的 ZnO@沸石咪唑酯骨架-8（ZIF-8）复合材料被报道为一种高效的光热催化剂，与母体 ZnO 纳米棒相比，它显示出更高的转化效率和高催化选择性和耐久性，用于连续乙醇氧化系统。ZnO@ZIF-8 复合材料对乙醛的产生具有 91.5% 的高选择性。使用电化学阻抗谱探测潜在机制，N 2吸附-解吸等温线、瞬态开路电位、稳态和时间分辨光致发光光谱。总的来说，探测表明改进的性能源于 1) 促进电荷分离；2)降低氧化电位空穴；3) 扩大表面积；4）优选的反应路线。这项工作为设计用于选择性太阳能转化为所需化学物质的混合光热催化剂提供了新的视角。
更新日期：2020-10-23
中文翻译：
在纳米结构沸石咪唑酯骨架-8 包裹的 ZnO 光热催化剂薄膜上选择性乙醇氧化成乙醛
光热催化乙醇氧化为乙醛为合成高附加值化学品提供了一种替代技术。然而，过度氧化导致完全矿化的竞争阻碍了实际应用。在此，一维纳米结构的 ZnO@沸石咪唑酯骨架-8（ZIF-8）复合材料被报道为一种高效的光热催化剂，与母体 ZnO 纳米棒相比，它显示出更高的转化效率和高催化选择性和耐久性，用于连续乙醇氧化系统。ZnO@ZIF-8 复合材料对乙醛的产生具有 91.5% 的高选择性。使用电化学阻抗谱探测潜在机制，N 2吸附-解吸等温线、瞬态开路电位、稳态和时间分辨光致发光光谱。总的来说，探测表明改进的性能源于 1) 促进电荷分离；2)降低氧化电位空穴；3) 扩大表面积；4）优选的反应路线。这项工作为设计用于选择性太阳能转化为所需化学物质的混合光热催化剂提供了新的视角。
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