Optimizing accuracy and efficacy in data-driven materials discovery for the solar production of hydrogen

Xiong, Yihuang; Campbell, Quinn; Fanghanel, Julian; Badding, Catherine K.; Wang, Huaiyu; Kirchner‐Hall, Nicole E.; Theibault, Monica J.; Timrov, Iurii; Mondschein, Jared; Seth, Kriti; Katz, Rebecca; Villarino, Andrés Molina; Pamuk, Betül; Penrod, Megan; Khan, Mohammed M.; Rivera, Tiffany; Smith, Nathan; Quintana, Xavier; Orbe, Paul; Fennie, Craig J.; Asem-Hiablie, Senorpe; Young, James L.; Deutsch, Todd G.; Cococcioni, Matteo; Gopalan, Venkatraman; Abruña, Héctor D.; Schaak, Raymond E.; Dabo, Ismaïla

doi:10.1039/d0ee02984j

Cited by 36 publications

(46 citation statements)

References 102 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Moreover, this work shows that DFT+U with Hubbard parameters determined nonempirically can be used to predict reliable band gaps at lower computational cost than that of hybrid functionals (such as HSE06 [96,97]) that are popular for predicting band gap values. This is important for high-throughput studies that require efficient and reliable estimates of the band gaps at moderate computational cost for various technologically relevant materials such as photocatalysts [98,99], solar cells [100,101], and transparent conductors [102].…”

Section: Introductionmentioning

confidence: 99%

Extensive Benchmarking of DFT+U Calculations for Predicting Band Gaps

et al. 2021

Self Cite

View full text Add to dashboard Cite

Accurate computational predictions of band gaps are of practical importance to the modeling and development of semiconductor technologies, such as (opto)electronic devices and photoelectrochemical cells. Among available electronic-structure methods, density-functional theory (DFT) with the Hubbard U correction (DFT+U) applied to band edge states is a computationally tractable approach to improve the accuracy of band gap predictions beyond that of DFT calculations based on (semi)local functionals. At variance with DFT approximations, which are not intended to describe optical band gaps and other excited-state properties, DFT+U can be interpreted as an approximate spectral-potential method when U is determined by imposing the piecewise linearity of the total energy with respect to electronic occupations in the Hubbard manifold (thus removing self-interaction errors in this subspace), thereby providing a (heuristic) justification for using DFT+U to predict band gaps. However, it is still frequent in the literature to determine the Hubbard U parameters semiempirically by tuning their values to reproduce experimental band gaps, which ultimately alters the description of other total-energy characteristics. Here, we present an extensive assessment of DFT+U band gaps computed using self-consistent ab initioU parameters obtained from density-functional perturbation theory to impose the aforementioned piecewise linearity of the total energy. The study is carried out on 20 compounds containing transition-metal or p-block (group III-IV) elements, including oxides, nitrides, sulfides, oxynitrides, and oxysulfides. By comparing DFT+U results obtained using nonorthogonalized and orthogonalized atomic orbitals as Hubbard projectors, we find that the predicted band gaps are extremely sensitive to the type of projector functions and that the orthogonalized projectors give the most accurate band gaps, in satisfactory agreement with experimental data. This work demonstrates that DFT+U may serve as a useful method for high-throughput workflows that require reliable band gap predictions at moderate computational cost.

show abstract

Section: Introductionmentioning

confidence: 99%

Extensive Benchmarking of DFT+U Calculations for Predicting Band Gaps

et al. 2021

Self Cite

View full text Add to dashboard Cite

show abstract

“…Electronic mail: vxg8@psu.edu cial applications 15 . Data driven prediction of new photocatalytic materials provides new opportunities for expediting the discovery and development of efficient photocatalysis 16 . Most of the reported photocatalysts require co-catalysts, sensitizers or support materials to reach above 0.1 µmol/h hydrogen production rate 14 .…”

Section: Introductionmentioning

confidence: 99%

“…This motivates our present work in building an ultra-sensitive tool for detecting small rates of hydrogen generation. Using this tool, we study the hydrogen evolution rates of two recently identified photocatalyst materials 16 .…”

Section: Introductionmentioning

confidence: 99%

“…The results from a pair of standard photocatalysts, namely, 0.3 wt% Pt loaded TiO 2 rutile phase and bare TiO 2 rutile phase are presented to demonstrate the working principles of the setup. Furthermore, the detection of hydrogen from three recently discovered candidates, Ca 2 PbO 4 , ZnFe 2 O 4 , and MgSb 2 O 6 16 , are presented to showcase the application in fast screening of predicted samples from first-principle calculation without co-catalyst or electrode. While the photocatalytic activity of ZnFe 2 O 4 has recently been investigated and optimized [20][21][22] , our literature search did not reveal previous experimental evidence of the photocatalytic activity of Ca 2 PbO 4 .…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Ultrasensitive electrode-free and co-catalyst-free detection of nanomoles per hour hydrogen evolution for the discovery of new photocatalysts

Wang

Katz

Fanghanel

et al. 2022

Review of Scientific Instruments

Self Cite

View full text Add to dashboard Cite

High throughput theoretical methods are increasingly used to identify promising photocatalytic materials for hydrogen generation from water as a clean source of energy. While most promising water splitting candidates require co-catalyst loading and electrical biasing, computational costs to predict them apriori becomes large. It is therefore important to identify bare, bias-free semiconductor photocatalysts with small initial hydrogen production rates, often in the range of tens of nano-mols per hour, as these can become highly efficient with further co-catalyst loading and biasing. Here we report a sensitive hydrogen detection system suitable for screening new photocatalysts. The hydrogen evolution rate of the prototypical rutile TiO 2 loaded with 0.3 % wt Pt is detected to be 78.0±0.8 µmol/h/0.04g, comparable with the rates reported in literature. In contrast, sensitivity to an ultralow evolution rate of 11.4±0.3 nmol/h/0.04g is demonstrated for bare polycrystalline TiO 2 without electrical bias. Two candidate photocatalysts, ZnFe 2 O 4 (18.1±0.2 nmol/h/0.04g) and Ca 2 PbO 4 (35.6±0.5 nmol/h/0.04g), without electrical bias or co-catalyst loading, are demonstrated to be potentially superior to bare TiO 2 . This work expands the techniques available for sensitive detection of photocatalytic processes towards much faster screening of new candidate photocatalytic materials in their bare state.

show abstract

“…These observations were very useful to conduct e.g. a DFT+U -based high-throughput search of novel materials for the photocatalytic water splitting [90]. In the current work, we go further and explore the accuracy of the extended DFT+U +V formulation for predicting band gaps and its sensitivity to the type of Hubbard projectors.…”

Section: Key Question Ismentioning

confidence: 90%

Importance of intersite Hubbard interactions in $β$-MnO$_2$: A first-principles DFT+$U$+$V$ study

Mahajan,

Timrov,

Marzari

et al. 2021

Preprint

Self Cite

View full text Add to dashboard Cite

We present a first-principles investigation of the structural, electronic, and magnetic properties of pyrolusite (β-MnO2) using conventional and extended Hubbard-corrected density-functional theory (DFT+U and DFT+U +V ). The onsite U and intersite V Hubbard parameters are computed using linear-response theory in the framework of density-functional perturbation theory. We show that while the inclusion of the onsite U is crucial to describe the localized nature of the Mn(3d) states, the intersite V is key to capture accurately the strong hybridization between neighboring Mn(3d) and O(2p) states. In this framework, we stabilize the simplified collinear antiferromagnetic (AFM) ordering (suggested by the Goodenough-Kanamori rule) that is commonly used as an approximation to the experimentally-observed noncollinear screw-type spiral magnetic ordering. A detailed investigation of the ferromagnetic and of other three collinear AFM spin configurations is also presented. The findings from Hubbard-corrected DFT are discussed using two kinds of Hubbard manifolds -nonorthogonalized and orthogonalized atomic orbitals -showing that special attention must be given to the choice of the Hubbard projectors, with orthogonalized manifolds providing more accurate results than nonorthogonalized ones within DFT+U +V . This work paves the way for future studies of complex transition-metal compounds containing strongly localized electrons in the presence of pronounced covalent interactions.

show abstract

Optimizing accuracy and efficacy in data-driven materials discovery for the solar production of hydrogen

Abstract: The production of hydrogen fuels, via water splitting, is of practical relevance for meeting global energy needs and mitigating the environmental consequences of fossil-fuel-based transportation. Water photoelectrolysis has been proposed...

Cited by 36 publications

References 102 publications

Extensive Benchmarking of DFT+U Calculations for Predicting Band Gaps

Extensive Benchmarking of DFT+U Calculations for Predicting Band Gaps

Ultrasensitive electrode-free and co-catalyst-free detection of nanomoles per hour hydrogen evolution for the discovery of new photocatalysts

Importance of intersite Hubbard interactions in $β$-MnO$_2$: A first-principles DFT+$U$+$V$ study

Contact Info

Product

Resources

About