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Donor-Acceptor Couples of Metal and Metal Oxides with Enriched Ni3+ Active Sites for Oxygen Evolution
Ni, Shan1,2; Qu, Hongnan2; Xing, Huifang1,2; Xu, Zihao1,2; Zhu, Xiangyang1,2; Yuan, Menglei1,2; Wang, Li2; Yu, Jiemiao2; Li, Yanqing2; Yang, Liangrong1,2
刊名ACS APPLIED MATERIALS & INTERFACES
2021-04-21
卷号13期号:15页码:17501-17510
关键词oxygen evolution reaction solid-state method strong electronic interaction high-valence Ni3+ decreased Fermi level
ISSN号1944-8244
DOI10.1021/acsami.1c00890
英文摘要Exploiting precious-metal-free and high-activity oxygen evolution reaction (OER) electrocatalysts has been in great demands toward many energy storage and conversion processes, for example, carbon dioxide reduction, metal-air batteries, and water splitting. In this study, the simple solid-state method is employed for coupling Ni (electron donors) with lower-Fermi-level MoO2 or WOx (electron acceptors) into donoracceptor ensembles with well-designed interfaces as robust electrocatalysts for OER. The resulting Ni/MoO2 and Ni/WOx electrocatalysts exhibit smaller overpotentials of 287 and 333 mV at 10 mA cm(-2) as well as smaller Tafel slopes of 51 and 65 mV/ dec, respectively, with respect to the single Ni, MoO2, WOx, and even the benchmark RuO2 in 1 M KOH. Specially, on account of a higher Fermi level of Ni in comparison with MoO2 and WOx, their strong electronic interaction results in directional interfacial electron transfer and increases the hole density over Ni, dramatically enriching the population of high-valence Ni3+ active sites and decreasing the Fermi level of Ni. The existence of Ni3+ can strengthen the chemisorption of OH-, and the downshift of the Ni Fermi level can significantly expedite migration of electrons toward the surface of catalysts during OER, thus synergistically boosting the OER catalytic performance. Furthermore, the inner Ni/MoO2 and Ni/WOx heterostructures and the electrochemically induced surface layers of oxides/hydroxides collectively boost the OER kinetics. This study highlights the importance of designing highly efficient OER electrocatalysts with high-valence active species (Ni3+) and better matched energy levels induced by the work function difference through interfacial engineering.
资助项目National Natural Science Foundation of China[21922814] ; National Natural Science Foundation of China[21676273] ; National Natural Science Foundation of China[21961160745] ; National Natural Science Foundation of China[31961133019] ; National Natural Science Foundation of China[21921005] ; Beijing Natural Science Foundation[2194086]
WOS关键词HIGHLY EFFICIENT ELECTROCATALYSTS ; HYDROGEN EVOLUTION ; RATIONAL DESIGN ; WATER OXIDATION ; SURFACE ; NANOSTRUCTURES ; NANOPARTICLES ; FUNDAMENTALS ; REDUCTION ; NANOWIRES
WOS研究方向Science & Technology - Other Topics ; Materials Science
语种英语
出版者AMER CHEMICAL SOC
WOS记录号WOS:000643578300033
资助机构National Natural Science Foundation of China ; Beijing Natural Science Foundation
内容类型期刊论文
源URL[http://ir.ipe.ac.cn/handle/122111/48904]  
专题中国科学院过程工程研究所
通讯作者Yang, Liangrong; Liu, Huizhou
作者单位1.Univ Chinese Acad Sci, Sch Chem Engn, Beijing 100049, Peoples R China
2.Chinese Acad Sci, Inst Proc Engn, CAS Key Lab Green Proc & Engn, State Key Lab Biochem Engn, Beijing 100190, Peoples R China
推荐引用方式
GB/T 7714
Ni, Shan,Qu, Hongnan,Xing, Huifang,et al. Donor-Acceptor Couples of Metal and Metal Oxides with Enriched Ni3+ Active Sites for Oxygen Evolution[J]. ACS APPLIED MATERIALS & INTERFACES,2021,13(15):17501-17510.
APA Ni, Shan.,Qu, Hongnan.,Xing, Huifang.,Xu, Zihao.,Zhu, Xiangyang.,...&Liu, Huizhou.(2021).Donor-Acceptor Couples of Metal and Metal Oxides with Enriched Ni3+ Active Sites for Oxygen Evolution.ACS APPLIED MATERIALS & INTERFACES,13(15),17501-17510.
MLA Ni, Shan,et al."Donor-Acceptor Couples of Metal and Metal Oxides with Enriched Ni3+ Active Sites for Oxygen Evolution".ACS APPLIED MATERIALS & INTERFACES 13.15(2021):17501-17510.
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