Orientational-growth of Cu2O {111} or {110} facets induced by frustules for CO2-H2O specific photo(electro)chemical conversion into methanol/ethanol under visible-light

IF 8.4 2区工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of CO2 Utilization Pub Date : 2025-05-01 Epub Date: 2025-03-27 DOI:10.1016/j.jcou.2025.103071

Michele Aresta , Tomasz Baran , Domenico Caringella , Shambel G. Wasse , Yusuf I. Abubakar , Alessandra Petrucciani , Alessandra Norici , Ernesto Mesto , Elvira De Giglio , Roberto Comparelli , Angela Dibenedetto

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Abstract

p-Type-semiconductor Cu₂O facets {111} (octahedral) and {110} (rhombododecahedral) present a higher photo(electro)catalytic activity towards CO2RRs (CO₂ Reduction Reaction) than {100} (cubic). Two frustules (the siliceous skeleton of microalgae Diatoms) having a different morphology, namely: Navicula sp. (Nsp, elongated pore-shape) and Conticribra weissflogii (Cw, round pore-shape) have been used for the first time in this work as template for the orientational growth of Cu₂O facets. Frustules are calcinated at 700 °C to avoid residual organics that may give false positives during photo(electro)catalysis. Each of the frustules is found to induce a facet of Cu₂O preferentially. Nsp induces the {111} facet (Band-gap=2.26 eV), while Cw preferentially induces the {110} facet (Band-gap=1.96 eV). Under visible light irradiation, Nsp-grown Cu₂O converts CO₂ and H₂O into methanol, while Cw-grown Cu₂O produces ethanol. The different behaviour is related to the different Cu-Cu distance (the active catalytic centres) in the two facets.

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Cu2O{111}或{110}晶圆在可见光下定向生长以实现CO2-H2O特异光（电）化学转化为甲醇/乙醇

p型半导体Cu2O切面{111}（八面体）和{110}（菱形十二面体）对CO2还原反应的光（电）催化活性高于{100}（立方）。本文首次采用两种不同形态的微藻硅藻硅质骨架：Navicula sp. （Nsp，细长孔形）和Conticribra weissflogii （Cw，圆孔形）作为Cu2O晶面定向生长的模板。在700°C下煅烧，以避免在光（电）催化过程中可能产生假阳性的残留有机物。研究发现，每一种晶体都优先诱导Cu2O的一个侧面。Nsp诱导{111}面（Band-gap=2.26 eV），而Cw优先诱导{110}面（Band-gap=1.96 eV）。在可见光照射下，nsp生长的Cu2O将CO2和H2O转化为甲醇，而cw生长的Cu2O则产生乙醇。不同的行为与两个方面不同的Cu-Cu距离（活性催化中心）有关。

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来源期刊

Journal of CO2 Utilization CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL

CiteScore

13.90

自引率

10.40%

发文量

406

审稿时长

2.8 months

期刊介绍： The Journal of CO2 Utilization offers a single, multi-disciplinary, scholarly platform for the exchange of novel research in the field of CO2 re-use for scientists and engineers in chemicals, fuels and materials. The emphasis is on the dissemination of leading-edge research from basic science to the development of new processes, technologies and applications. The Journal of CO2 Utilization publishes original peer-reviewed research papers, reviews, and short communications, including experimental and theoretical work, and analytical models and simulations.