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原位构建具有光热和相互催化作用的界面用于高效太阳能驱动的MgH可逆储氢

In Situ Construction of Interface with Photothermal and Mutual Catalytic Effect for Efficient Solar-Driven Reversible Hydrogen Storage of MgH.

作者信息

Hu Xuechun, Chen Xiaowei, Zhang Xiaoyue, Meng Yang, Xia Guanglin, Yu Xuebin, Sun Dalin, Fang Fang

机构信息

Department of Materials Science, Fudan University, Shanghai, 200433, P. R. China.

Department of Physics, Jimei University, Xiamen, 361021, P. R. China.

出版信息

Adv Sci (Weinh). 2024 Jun;11(22):e2400274. doi: 10.1002/advs.202400274. Epub 2024 Mar 22.

Abstract

Hydrogen storage in MgH is an ideal solution for realizing the safe storage of hydrogen. High operating temperature, however, is required for hydrogen storage of MgH induced by high thermodynamic stability and kinetic barrier. Herein, flower-like microspheres uniformly constructed by N-doped TiO nanosheets coated with TiN nanoparticles are fabricated to integrate the light absorber and thermo-chemical catalysts at a nanometer scale for driving hydrogen storage of MgH using solar energy. N-doped TiO is in situ transformed into TiNO and Ti/TiH uniformly distributed inside of TiN matrix during cycling, in which TiN and Ti/TiH pairs serve as light absorbers that exhibit strong localized surface plasmon resonance effect with full-spectrum light absorbance capability. On the other hand, it is theoretically and experimentally demonstrated that the intimate interface between TiH and MgH can not only thermodynamically and kinetically promote H desorption from MgH but also simultaneously weaken Ti─H bonds and hence in turn improve H desorption from the combination of weakened Ti─H and Ti─H bonds. The uniform integration of photothermal and catalytic effect leads to the direct action of localized heat generated from TiN on initiating the catalytic effect in realizing hydrogen storage of MgH with a capacity of 6.1 wt.% under 27 sun.

摘要

MgH₂中的储氢是实现氢气安全储存的理想解决方案。然而,由于MgH₂具有高热力学稳定性和动力学势垒,其储氢需要较高的操作温度。在此,制备了由涂覆有TiN纳米颗粒的N掺杂TiO₂纳米片均匀构建的花状微球,以在纳米尺度上整合光吸收剂和热化学催化剂,从而利用太阳能驱动MgH₂的储氢。在循环过程中,N掺杂TiO₂原位转变为TiNO和均匀分布在TiN基体内部的Ti/TiH,其中TiN和Ti/TiH对作为光吸收剂,表现出强烈的局域表面等离子体共振效应,具有全光谱光吸收能力。另一方面,理论和实验证明,TiH与MgH₂之间的紧密界面不仅可以在热力学和动力学上促进MgH₂中H的解吸,还可以同时削弱Ti─H键,进而改善从减弱的Ti─H和Ti─H键组合中H的解吸。光热效应和催化效应的均匀整合导致TiN产生的局部热量直接作用于引发催化效应,从而在27个太阳光照下实现容量为6.1 wt.%的MgH₂储氢。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/76b3/11165547/00706c02cd7a/ADVS-11-2400274-g006.jpg

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