ZnO HoMS@ZIF-8 Nanoreactors for Efficient Enrichment and Photoreduction of Atmospheric CO_(2)  

作　　者：Yanze Wei Juan Li Decai Zhao Yasong Zhao Qinghua Zhang Lin Gu Jiawei Wan Dan Wang 

机构地区：[1]State Key Laboratory of Biochemical Engineering,Institute of Process Engineering,Chinese Academy of Sciences,Beijing 100190 [2]Key Laboratory of Biopharmaceutical Preparation and Delivery,Chinese Academy of Sciences,Beijing 100190 [3]University of Chinese Academy of Sciences,Beijing 100049 [4]Beijing National Laboratory for Condensed Matter Physics,Institute of Physics,Chinese Academy of Sciences,Beijing 100190

出　　处：《CCS Chemistry》2024年第12期3065-3076,共12页中国化学会会刊(英文)

基　　金：supported by National Natural Science Foundation of China(grant nos.21821005,21931012,21820102002,22293043,52272097,and 52202354);the Beijing Natural Science Foundation(grant no.2242019);the DNL Cooperation Fund,Chinese Academy of Sciences(CAS)(grant no.DNL202020).

摘　　要：The ultimate goal of photocatalytic CO_(2)reduction is to efficiently convert atmospheric CO_(2)into value-added products by designing hierarchical photocatalysts that combine effective harvesting and accelerate activation capabilities of CO_(2)molecules.In this work,we demonstrated direct air-level CO_(2)reduction by hollow multishell structure(HoMS)nanoreactors with zeolitic imidazolate framework-8(ZIF-8)-modified ZnO heteroshells,which offers a promising solution to optimize the mass transfer process via selective sieving and effective enrichment of CO_(2)molecules from the atmospheric environments.Specifically,heteroshells with ZIF-8 matrix act as pumps that effectively capture CO_(2)molecules,while the cavities serve as tanks to hold these molecules,thus significantly enhancing the transfer kinetics for CO_(2)photoreduction.The periodic shell-cavity configuration allows the nanoreactor to effectively gather CO_(2)molecules near the catalytic sites,thus increasing conversion opportunities for activated molecules.Simultaneously,the surface atomic steps on the ZnO/ZIF-8 heterointerfaces with staggered geometry expedite charge transfer and adsorption efficiency,which synergistically boosts the CO_(2)-CO yield up to 3.7μmol/h under CO_(2)flow and 0.7μmol/h under atmospheric conditions with almost complete CO selectivity.Hopefully,the HoMS nanoreactors offer a potential strategy for solving the“last mile”challenge in practical CO_(2)valorization.

关 键 词：hollow multishelled structures atmospheric CO_(2)photoreduction ZNO ZIF-8 HETEROINTERFACE 

分 类 号：O64[理学—物理化学]