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1.
Angew Chem Int Ed Engl ; 63(2): e202314099, 2024 Jan 08.
Article in English | MEDLINE | ID: mdl-38059828

ABSTRACT

Zn-based catalysts hold great potential to replace the noble metal-based ones for CO2 reduction reaction (CO2 RR). Undercoordinated Zn (Znδ+ ) sites may serve as the active sites for enhanced CO production by optimizing the binding energy of *COOH intermediates. However, there is relatively less exploration into the dynamic evolution and stability of Znδ+ sites during CO2 reduction process. Herein, we present ZnO, Znδ+ /ZnO and Zn as catalysts by varying the applied reduction potential. Theoretical studies reveal that Znδ+ sites could suppress HER and HCOOH production to induce CO generation. And Znδ+ /ZnO presents the highest CO selectivity (FECO 70.9 % at -1.48 V vs. RHE) compared to Zn and ZnO. Furthermore, we propose a CeO2 nanotube with confinement effect and Ce3+ /Ce4+ redox to stabilize Znδ+ species. The hollow core-shell structure of the Znδ+ /ZnO/CeO2 catalyst enables to extremely expose electrochemically active area while maintaining the Znδ+ sites with long-time stability. Certainly, the target catalyst affords a FECO of 76.9 % at -1.08 V vs. RHE and no significant decay of CO selectivity in excess of 18 h.

2.
ACS Appl Mater Interfaces ; 13(19): 22495-22504, 2021 May 19.
Article in English | MEDLINE | ID: mdl-33969687

ABSTRACT

Optically transparent wood has emerged as a promising glazing material. Thanks to the high optical transmittance, strong mechanical properties, and excellent thermal insulation capability of transparent wood, it offers a potential alternative to glass for window applications. Recently, thermo-, electro-, and photochromic transparent woods that dynamically modulate light transmittance have been investigated to improve building energy efficiency. However, it remains challenging to widely replace windows with transparent wood because of its poor weather resistance. In this study, an environment-friendly thermochromic transparent wood film (TTWF) with thermal switching of transmittance is proposed and demonstrated. To achieve thermochromism, the bleached wood is impregnated with the vanadium dioxide (VO2)/polyvinyl alcohol composite. Due to the self-densification of cellulose microfibrils during the evaporation of solvents, the transparent wood is in the form of thin films, which can be attached on the inner face of a window to protect it from severe weather conditions, making the installation convenient and low-cost. Furthermore, the surface of VO2-TTWF is modified by octadecyltrichlorosilane to enhance the waterproof ability and achieve self-cleaning and antidust functions. The proposed VO2-TTWF shows great potential for application in energy-efficient buildings using sustainable materials with advanced optical properties (i.e., Tlum = 50.5%, ΔTsol = 3.4%, and haze = 70%) that are mechanically robust (i.e., σ = 130.6 MPa along the wood growth direction), have low-thermal conductivity (i.e., K = 0.29 W m-1 K-1 along the perpendicular direction to the wood fibers), and demonstrate hydrophobic self-cleaning and antidust functions (i.e., contact angle: 121.9°). An experiment, using a model house, showed that the VO2-TTWF attached on the inner face of the window could significantly reduce the indoor air temperature by 33.9 °C compared with a bare glass panel, proving that VO2-TTWF has potential to be applied as a new-generation energy-efficient material for smart windows.

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