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一种对MgH₂中储氢具有高催化活性的新型CeFeZrO固溶体。

A novel CeFeZrO solid solution with high catalytic activity for hydrogen storage in MgH.

作者信息

Cheng Ying, Zhou Shuhua, Shi Biqing, Dong Bing, Ji Xianbin, Li Siqi, Zhang Wei

机构信息

Department of Environmental Engineering, Hebei University of Environmental Engineering Qinhuangdao 066102 PR China.

Hebei Key Laboratory of Applied Chemistry, School of Environmental and Chemical Engineering, Yanshan University Qinhuangdao 066004 PR China

出版信息

RSC Adv. 2021 Nov 23;11(60):37677-37683. doi: 10.1039/d1ra06951a.

DOI:10.1039/d1ra06951a
PMID:35498102
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9043827/
Abstract

The effect of the solid solution CeFeZrO, successfully prepared by a hydrothermal synthesis method, on the hydrogen sorption properties of MgH is systemically investigated. The CeFeZrO-modified MgH composite exhibits remarkable hydrogen kinetics properties and thermodynamics behavior compared to those of as-milled MgH, with a reduction in the initial desorption temperature of approximately 82 K. With respect to the hydrogen kinetics, the CeFeZrO-added sample could uptake approximately 5.3 wt% H at 473 K in 2500 s, whereas only 1.5 wt% hydrogen could be absorbed by pristine MgH in the same conditions. Furthermore, about 4.5 wt% of hydrogen could be desorbed by CeFeZrO-doped MgH composite at 623 K, which was 2 wt% higher than the as-milled MgH sample over the same period of time. The decomposition apparent activation energy for MgH-CeFeZrO is reduced to 84.3 kJ mol, which is about 77 kJ mol lower than that of pristine MgH. It is believed that the notable improvement in the hydrogen sorption kinetics is due to the -formed active species of CeH and MgO as well as the abundant oxygen vacancies, which play a vital role in catalyzing the hydrogen sorption performance of MgH.

摘要

通过水热合成法成功制备的固溶体CeFeZrO对MgH储氢性能的影响进行了系统研究。与球磨后的MgH相比,CeFeZrO改性的MgH复合材料表现出显著的氢动力学性能和热力学行为,初始脱附温度降低了约82 K。在氢动力学方面,添加CeFeZrO的样品在473 K下2500 s内可吸收约5.3 wt%的H,而在相同条件下原始MgH仅能吸收1.5 wt%的氢。此外,CeFeZrO掺杂的MgH复合材料在623 K下可解吸约4.5 wt%的氢,比球磨后的MgH样品在同一时间段内高2 wt%。MgH-CeFeZrO的分解表观活化能降低至84.3 kJ/mol,比原始MgH低约77 kJ/mol。据信,氢吸附动力学的显著改善归因于形成的活性物种CeH和MgO以及丰富的氧空位,它们在催化MgH的氢吸附性能方面起着至关重要的作用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f8bb/9043827/cb83a221bf5f/d1ra06951a-f8.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f8bb/9043827/7326f4ea1624/d1ra06951a-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f8bb/9043827/1628041d95bb/d1ra06951a-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f8bb/9043827/520aebd49007/d1ra06951a-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f8bb/9043827/cb83a221bf5f/d1ra06951a-f8.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f8bb/9043827/f5688933e621/d1ra06951a-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f8bb/9043827/5e0f610b42ee/d1ra06951a-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f8bb/9043827/4d6fb4b9e247/d1ra06951a-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f8bb/9043827/df30d5e60b05/d1ra06951a-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f8bb/9043827/7326f4ea1624/d1ra06951a-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f8bb/9043827/1628041d95bb/d1ra06951a-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f8bb/9043827/520aebd49007/d1ra06951a-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f8bb/9043827/cb83a221bf5f/d1ra06951a-f8.jpg

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本文引用的文献

1
Nanolayer-like-shaped MgFeO synthesised a simple hydrothermal method and its catalytic effect on the hydrogen storage properties of MgH.通过一种简单的水热法合成的纳米层状MgFeO及其对MgH储氢性能的催化作用。
RSC Adv. 2018 Apr 25;8(28):15667-15674. doi: 10.1039/c8ra02168f. eCollection 2018 Apr 23.
2
Reversible interconversion between methanol-diamine and diamide for hydrogen storage based on manganese catalyzed (de)hydrogenation.基于锰催化(脱)氢化作用的甲醇二胺与二酰胺之间的可逆相互转化用于储氢
Nat Commun. 2020 Jan 30;11(1):591. doi: 10.1038/s41467-020-14380-3.
3
A new 3DOM Ce-Fe-Ti material for simultaneously catalytic removal of PM and NOx from diesel engines.
一种新型 3DOM Ce-Fe-Ti 材料,用于同时催化去除柴油机中的 PM 和 NOx。
J Hazard Mater. 2018 Jan 15;342:317-325. doi: 10.1016/j.jhazmat.2017.08.040. Epub 2017 Aug 18.
4
Simultaneous NO and Particulate Matter Removal from Diesel Exhaust by Hierarchical Fe-Doped Ce-Zr Oxide.通过分级铁掺杂铈锆氧化物同时去除柴油机尾气中的氮氧化物和颗粒物
ACS Catal. 2017 Jun 2;7(6):3883-3892. doi: 10.1021/acscatal.6b03387. Epub 2017 Apr 26.