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	Charge carrier transport dynamics in w/mo-doped bivo4: first principles-based mesoscale characterization
	Pasumarthi, Viswanath1; Liu, Taifeng2; Dupuis, Michel1,3,4; Li, Can4,5
刊名	Journal of materials chemistry a
	2019-02-21
卷号	7期号:7页码:3054-3065
ISSN号	2050-7488
DOI	10.1039/c8ta09899a
通讯作者	Liu, taifeng(tfliu@vip.henu.edu.cn) ; Dupuis, michel(mdupuis2@buffalo.edu)
英文摘要	We present mesoscale characterization of carrier transport in w/mo-doped ms-bivo4 (bvo) to supplement our earlier study of electron and hole transport in bulk bvo. the mesoscale kinetic monte carlo (kmc) approach, supported by first principles-determined electron and hole hopping rates, captures the complex dynamics of electron carriers arising from light absorption and from metal doping. the computations and simulations support the observation that, for the doping level used in experiment, doping atoms do not affect significantly the transport dynamics of the charge carriers compared to stoichiometric bvo. w/mo doping increases the electron carrier concentration and consequently the electrode conductivity. we used a density functional theory dft + u method to characterize the electronic structure of doped bvo. each w and mo atom brings one more valence electron than a v atom. these excess electrons are mobile. we adopted the theories and methods of our earlier investigations on bvo. the dft + u theory affords an accurate description of small electron polarons with electrons localized on w or mo or v, as well as of the hopping barriers from w/mo-to-v or v-to-v. calculations on a 3 x 3 x 1 supercell of w/mo-doped ms-bvo indicate that the excess electron from w or mo does not reside on the doping atom. there is a shallow interaction region around the doping atom where the excess electron localized on a v atom is more stable than when localized on the doping atom and slightly more stable than when the excess electron is localized far away from the doping atom. this region is two nearest v atom-wide for w and three nearest atom-wide for mo. the depths of these stabilization regions are very small, similar to-0.65 k(b)t (at 300 k) for w and similar to-0.73 k(b)t for mo. calculated v-to-v hopping barriers in the doped material are little affected within the region and not affected outside the region. using our recently developed lattice-based kinetic monte carlo code adapted to account for doping atoms and their energy stabilization regions, we calculated the diffusivity of electrons for carrier density relevant to experiment as well as the conductivity. the stabilization regions have little effect on the diffusivity compared to the stoichiometric system because of the smallness of the stabilization. the diffusivity is found to decrease slightly with an increasing number of carriers, but the conductivity of a system with electron polarons arising from doping together with light absorption increases compared to that of the un-doped system. this work will set the foundation to study electron transport in gradient (w/mo)-doped systems and other mixed phase systems.
WOS关键词	KINETIC MONTE-CARLO ; SCANNING ELECTROCHEMICAL MICROSCOPY ; TOTAL-ENERGY CALCULATIONS ; SMALL-POLARON ; ADIABATIC THEORY ; OXIDE ; PHOTOANODES ; CATALYSTS ; MOBILITY ; MO
WOS研究方向	Chemistry ; Energy & Fuels ; Materials Science
WOS类目	Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000458682100053
内容类型	期刊论文
URI标识	http://www.corc.org.cn/handle/1471x/2372792
专题	大连化学物理研究所
通讯作者	Liu, Taifeng; Dupuis, Michel
作者单位	1.SUNY Buffalo, Dept Chem & Biol Engn, Buffalo, NY 14260 USA 2.Henan Univ, Collaborat Innovat Ctr Nano Funct Mat & Applicat, Natl & Local Joint Engn Res Ctr Appl Technol Hybr, Kaifeng 475004, Peoples R China 3.SUNY Buffalo, Computat & Data Enabled Sci & Engn Program, Buffalo, NY 14260 USA 4.Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian, Peoples R China 5.Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian, Peoples R China
推荐引用方式 GB/T 7714	Pasumarthi, Viswanath,Liu, Taifeng,Dupuis, Michel,et al. Charge carrier transport dynamics in w/mo-doped bivo4: first principles-based mesoscale characterization[J]. Journal of materials chemistry a,2019,7(7):3054-3065.
APA	Pasumarthi, Viswanath,Liu, Taifeng,Dupuis, Michel,&Li, Can.(2019).Charge carrier transport dynamics in w/mo-doped bivo4: first principles-based mesoscale characterization.Journal of materials chemistry a,7(7),3054-3065.
MLA	Pasumarthi, Viswanath,et al."Charge carrier transport dynamics in w/mo-doped bivo4: first principles-based mesoscale characterization".Journal of materials chemistry a 7.7(2019):3054-3065.

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