气候变化领域集成服务门户(CCPortal): Operando unraveling photothermal-promoted dynamic active-sites generation in NiFe2O4 for markedly enhanced oxygen evolution

CCPortal

DOI	10.1073/pnas.2023421118
	Operando unraveling photothermal-promoted dynamic active-sites generation in NiFe2O4 for markedly enhanced oxygen evolution
	Gao L.; Cui X.; Wang Z.; Sewell C.D.; Li Z.; Liang S.; Zhang M.; Li J.; Hu Y.; Lin Z.
发表日期	2021
ISSN	00278424
卷号	118 期号:7
英文摘要	The ability to develop highly active and low-cost electrocatalysts represents an important endeavor toward accelerating sluggish water-oxidation kinetics. Herein, we report the implementation and unraveling of the photothermal effect of spinel nanoparticles (NPs) on promoting dynamic active-sites generation to markedly enhance their oxygen evolution reaction (OER) activity via an integrated operando Raman and density functional theory (DFT) study. Specifically, NiFe2O4 (NFO) NPs are first synthesized by capitalizing on amphiphilic star-like diblock copolymers as nanoreactors. Upon the near-infrared light irradiation, the photothermal heating of the NFO-based electrode progressively raises the temperature, accompanied by a marked decrease of overpotential. Accordingly, only an overpotential of 309 mV is required to yield a high current density of 100 mA cm−2, greatly lower than recently reported earth-abundant electrocatalysts. More importantly, the photothermal effect of NFO NPs facilitates surface reconstruction into high-active oxyhydroxides at lower potential (1.36 V) under OER conditions, as revealed by operando Raman spectroelectrochemistry. The DFT calculation corroborates that these reconstructed (Ni,Fe)oxyhydroxides are electrocatalytically active sites as the kinetics barrier is largely reduced over pure NFO without surface reconstruction. Given the diversity of materials (metal oxides, sulfides, phosphides, etc.) possessing the photo-to-thermal conversion, this effect may thus provide a unique and robust platform to boost highly active surface species in nanomaterials for a fundamental understanding of enhanced performance that may underpin future advances in electrocatalysis, photocatalysis, solar-energy conversion, and renewable-energy production. © 2021 National Academy of Sciences. All rights reserved.
英文关键词	Nanoreactor \| photothermal effect \| operando Raman \| dynamic surface reconstruction \| density functional theory
语种	英语
scopus关键词	amphophile; copolymer; hydroxide; iron; metal oxide; nanomaterial; nanoparticle; nickel; oxygen; oxyhydroxide; phosphine; sulfide; unclassified drug; Article; catalyst; current density; density functional theory; electrocatalyst; energy conversion; energy yield; high temperature procedures; light irradiance; mathematical model; oxygen evolution; photocatalysis; photothermal effect; priority journal; Raman spectrometry; renewable energy; synthesis
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/180649
作者单位	School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, GA 30332, United States; Key Laboratory of Bio‐based Material Science and Technology of Ministry of Education, Northeast Forestry University, Harbin, 150040, China; Nanjing Key Laboratory of Advanced Functional Materials, Nanjing Xiaozhuang University, Nanjing, 211171, China
推荐引用方式 GB/T 7714	Gao L.,Cui X.,Wang Z.,et al. Operando unraveling photothermal-promoted dynamic active-sites generation in NiFe2O4 for markedly enhanced oxygen evolution[J],2021,118(7).
APA	Gao L..,Cui X..,Wang Z..,Sewell C.D..,Li Z..,...&Lin Z..(2021).Operando unraveling photothermal-promoted dynamic active-sites generation in NiFe2O4 for markedly enhanced oxygen evolution.Proceedings of the National Academy of Sciences of the United States of America,118(7).
MLA	Gao L.,et al."Operando unraveling photothermal-promoted dynamic active-sites generation in NiFe2O4 for markedly enhanced oxygen evolution".Proceedings of the National Academy of Sciences of the United States of America 118.7(2021).