A Blueprint for Photocatalytic Water Splitting: Mapping Multidimensional Compositional Space to Simultaneously Optimize Thermodynamics and Kinetics

Sunlight is a vast source of renewable energy but its intermittent nature means that its utilization requires a means of storing this energy. One attractive approach for solar energy storage is to harness the energy of sunlight to split water into hydrogen and oxygen i.e. solar generated fuels. The solar generated fuels can be combusted to release energy efficiently with water as the only by-product. As a result, this approach avoids the deleterious consequences of greenhouse emissions that accompany the combustion of conventional fossil fuels. The complex cascade of reactions required to harvest sunlight and split water into hydrogen and oxygen present a formidable scientific challenge. The project seeks to develop hybrid materials as the catalyst for water splitting, such that individual components are assembled and function synergistically. The project further works towards employing components that are highly tunable in terms of their energy levels, thereby providing a versatile platform that can be optimized for converting sunlight and water into fuel. Employing a judicious mix of calculations from supercomputers and selective experiments accelerates the rational design of materials for efficient solar energy storage within chemical bonds. The project team mentors young scientists from underrepresented groups and engages K-12 students and teachers in activities that emphasize the opportunities made available by big data and solar energy.

Publications

Photocatalytic hydrogen evolution mechanisms mediated by stereoactive lone pairs of Sb2VO5 in quantum dot heterostructures

W. Zaheer, C. R. McGranahan, J. R. Ayala, K. Garcia-Pedraza, L. J. Carrillo, A. R. M. Rothfuss, U. Wijethunga, G. Agbeworvi, A. R. Giem, J. L. Andrews, J. V. Handy, S. Perez-Beltran, R. Calderon-Oliver, L. Ma, S. N. Ehrlich, C. Jaye, C. Weiland, D. A. Fischer, D. F. Watson, and S. Banerjee

1/1/2024

Ultrafast Charge Transfer Enhancement in CdS–MoS₂ via a Linker Molecule

M. Ciesler, H. Wang, S. Zhang, and D. West

9/22/2023

Linker-Assisted Assembly of Ligand-Bridged CdS/MoS₂ Heterostructures: Tunable Light-Harvesting Properties and Ligand-Dependent Control of Charge-Transfer Dynamics and Photocatalytic Hydrogen Evolution

A. R. M. Rothfuss, J. R. Ayala, J. V. Handy, C. R. McGranahan, K. E. García-Pedraza, S. Banerjee, and D. F. Watson

8/10/2023

Effect of Stereochemically Active Electron Lone Pairs on Magnetic Ordering in Trivanadates

G. Agbeworvi, W. Zaheer, J. D. Ponis, J. V. Handy, J. R. Ayala, J. L. Andrews, P. Schofield, C. Jaye, C. Weiland, D. A. Fischer, and S. Banerjee

8/2/2023

Giant excitonic effects in vacancy-ordered double perovskites

F. Zhang, W. Gao, G. J. Cruz, Y. Sun, P. Zhang, and J. Zhao

6/9/2023

Stacking up Electron-Rich and Electron-Deficient Monolayers to Achieve Extraordinary Mid- to Far-Infrared Excitonic Absorption: Interlayer Excitons in the C3B/C3N Bilayer

Z. Tang, G. J. Cruz, F. Jia, Y. Wu, W. Xia, and P. Zhang

4/27/2023

Multivariate hyperspectral data analytics across length scales to probe compositional, phase, and strain heterogeneities in electrode materials

D. A. Santos, J. L. Andrews, B. Lin, L. R. De Jesus, Y. Luo, S. Pas, M. A. Gross, L. Carillo, P. Stein, Y. Ding, B. Xu, and S. Banerjee

12/1/2022

Exploiting the stereoelectronic effects for selective tuning of band edge states of α-SnO: GW quasiparticle calculations

Y. Wu, Z. Tang, G. J. Cruz, Y. Yang, W. Zhang, W. Ren, and P. Zhang

8/1/2022

Thermodynamics of Wettability: A Physical Chemistry Laboratory Experiment

R. D. Davidson, T. E. O’Loughlin, T. E. G. Alivio, S. Lim, and S. Banerjee

6/28/2022

Prediction of protected band edge states and dielectric tunable quasiparticle and excitonic properties of monolayer MoSi2N4

Y. Wu, Z. Tang, W. Xia, W. Gao, F. Jia, Y. Zhang, W. Zhu, W. Zhang, and P. Zhang

6/15/2022

Nanostructured block copolymer muscles

C. Lang, E. C. Lloyd, K. E. Matuszewski, Y. Xu, V. Ganesan, R. Huang, M. Kumar, and R. J. Hickey

6/2/2022

Numerical methods for efficient GW calculations and the applications in low-dimensional systems

W. Gao, W. Xia, P. Zhang, J. R Chelikowsky, and J. Zhao

6/1/2022

A deep learned nanowire segmentation model using synthetic data augmentation

B. Lin, N. Emami, D. A. Santos, Y. Luo, S. Banerjee, and B. Xu

4/28/2022

Giant Narrow-Band Optical Absorption and Distinctive Excitonic Structures of Monolayer C3N and C3B

Z. Tang, G. J. Cruz, Y. Wu, W. Xia, F. Jia, W. Zhang, and P. Zhang

3/28/2022

High-Stability Light-Element Magnetic Superatoms Determined by Hund’s Rule

X. Wu, F. Yu, W. Xie, Z. Liu, Z. Wang, and S. Zhang

3/17/2022

Ultrahigh Photocatalytic CO₂ Reduction Efficiency and Selectivity Manipulation by Single‐Tungsten‐Atom Oxide at the Atomic Step of TiO₂

Y. Feng, C. Wang, P. Cui, C. Li, B. Zhang, L. Gan, S. Zhang, X. Zhang, X. Zhou, Z. Sun, K. Wang, Y. Duan, H. Li, K. Zhou, H. Huang, A. Li, C. Zhuang, L. Wang, Z. Zhang, and X. Han

3/17/2022

Lone but Not Alone: Precise Positioning of Lone Pairs for the Design of Photocatalytic Architectures

J. V. Handy, W. Zaheer, A. R. M. Rothfuss, C. R. McGranahan, G. Agbeworvi, J. L. Andrews, K. E. García-Pedraza, J. D. Ponis, J. R. Ayala, Y. Ding, D. F. Watson, and S. Banerjee

1/31/2022

Ligand-Assisted Charge-Transfer Mechanism: The Case of CdSe/Cysteine/MoS₂ Heterostructures

M. Ciesler, D. West, and S. Zhang

12/22/2021

Quasiparticle band structures of the 4d perovskite oxides SrZrO3 and BaZrO3

G. Lopez-Candales, Z. Tang, G. J. Cruz, W. Xia, F. Jia, and P. Zhang

11/15/2021

Electronic structure modulation of MoS2 by substitutional Se incorporation and interfacial MoO3 hybridization: Implications of Fermi engineering for electrocatalytic hydrogen evolution and oxygen evolution

A. Parija, W. Zaheer, J. Cho, T. E. G. Alivio, S. C. Fakra, M. Al-Hashimi, D. Prendergast, and S. Banerjee

3/1/2021

Quasiparticle band structure of SrTiO3 and BaTiO3 : A combined LDA+U and G0W0 approach

G. Lopez-Candales, Z. Tang, W. Xia, F. Jia, and P. Zhang

1/19/2021

Dual-stage K⁺ ion intercalation in V₂O₅-conductive polymer composites

D. S. Charles, F. Guo, X. Shan, S. Kim, Z. W. Lebens-Higgins, W. Xu, D. Su, L. F. J. Piper, and X. Teng

1/1/2021

Isosymmetric phase transitions, ultrahigh ductility, and topological nodal lines in α−Ag2S

Y. Liang, A. S. Ahmad, J. Zhao, G. Song, X. Zhou, J. Ji, W. Zhang, Z. Han, J. Liu, K. Stahl, A. Pakhomova, K. Glazyrin, G. Zhang, W. Zhang, Y. Zhao, R. Yu, S. Wang, and P. Zhang

10/15/2020

Elucidating the Mechanistic Origins of Photocatalytic Hydrogen Evolution Mediated by MoS₂/CdS Quantum-Dot Heterostructures

J. Cho, N. S. Suwandaratne, S. Razek, Y. Choi, L. F. J. Piper, D. F. Watson, and S. Banerjee

8/31/2020

Combined subsampling and analytical integration for efficient large-scale GW calculations for 2D systems

W. Xia, W. Gao, G. Lopez-Candales, Y. Wu, W. Ren, W. Zhang, and P. Zhang

8/6/2020

Lattice Anharmonicity of Stereochemically Active Lone Pairs Controls Thermochromic Band Gap Reduction of PbVO₃Cl

U. Dang, W. Zaheer, W. Zhou, A. Kandel, M. Orr, R. W. Schwenz, G. Laurita, S. Banerjee, and R. T. Macaluso

7/28/2020

Remarkable Band-Gap Renormalization via Dimensionality of the Layered Material C3B

Y. Wu, W. Xia, Y. Zhang, W. Zhu, W. Zhang, and P. Zhang

7/23/2020

Carrier Dynamics and Transfer across the CdS/MoS₂ Interface upon Optical Excitation

K. Cheng, H. Wang, J. Bang, D. West, J. Zhao, and S. Zhang

7/22/2020

High-Fidelity Transfer of Chemical Vapor Deposition Grown 2D Transition Metal Dichalcogenides via Substrate Decoupling and Polymer/Small Molecule Composite

P. Wang, S. Song, A. Najafi, C. Huai, P. Zhang, Y. Hou, S. Huang, and H. Zeng

5/18/2020

Designing catalysts for water splitting based on electronic structure considerations

S. A. Razek, M. R. Popeil, L. Wangoh, J. Rana, N. Suwandaratne, J. L. Andrews, D. F. Watson, S. Banerjee, and L. F. J. Piper

4/17/2020

Benchmarking PBE+D3 and SCAN+rVV10 methods using potential energy surfaces generated with MP2+ΔCCSD(T) calculation

J. Chen, W. Xie, K. Li, S. Zhang, and Y. Sun

1/1/2020

Navigating the design space of inorganic materials synthesis using statistical methods and machine learning

E. J. Braham, R. D. Davidson, M. Al-Hashimi, R. Arróyave, and S. Banerjee

1/1/2020

Flexible crystalline β-Ga₂O₃solar-blind photodetectors

J. Lai, M. N. Hasan, E. Swinnich, Z. Tang, S. Shin, M. Kim, P. Zhang, and J. Seo

1/1/2020

Type-II heterostructures of α-V2O5 nanowires interfaced with cadmium chalcogenide quantum dots: Programmable energetic offsets, ultrafast charge transfer, and photocatalytic hydrogen evolution

S. Chauhan, A. Sheng, J. Cho, S. A. Razek, N. Suwandaratne, M. Y. Sfeir, L. F. J. Piper, S. Banerjee, and D. F. Watson

12/9/2019

Ultrahigh Photocatalytic Rate at a Single‐Metal‐Atom‐Oxide

C. Wang, A. Li, C. Li, S. Zhang, H. Li, X. Zhou, L. Hu, Y. Feng, K. Wang, Z. Zhu, R. Shao, Y. Chen, P. Gao, S. Mao, J. Huang, Z. Zhang, and X. Han

11/14/2019

Structural water and disordered structure promote aqueous sodium-ion energy storage in sodium-birnessite

X. Shan, F. Guo, D. S. Charles, Z. Lebens-Higgins, S. Abdel Razek, J. Wu, W. Xu, W. Yang, K. L. Page, J. C. Neuefeind, M. Feygenson, L. F. J. Piper, and X. Teng

10/31/2019

Strain in van der Waals epitaxy and evidence for a collective macroscopic effect of a negligibly small perturbation

Z. Zhu, P. Cui, Y. Jia, S. Zhang, and Z. Zhang

7/22/2019

Tunable Type-II BiVO4/g - C3N4 Nanoheterostructures for Photocatalysis Applications

J. Zhang, M. Deng, Y. Yan, T. Xiao, W. Ren, and P. Zhang

4/17/2019

Machine Learning-Directed Navigation of Synthetic Design Space: A Statistical Learning Approach to Controlling the Synthesis of Perovskite Halide Nanoplatelets in the Quantum-Confined Regime

E. J. Braham, J. Cho, K. M. Forlano, D. F. Watson, R. Arròyave, and S. Banerjee

4/11/2019

Prediction of Ti3C2O2 MXene as an effective capturer of formaldehyde

Y. Zhang, Z. Zhou, J. Lan, and P. Zhang

3/1/2019

Prediction of MXene based 2D tunable band gap semiconductors: GW quasiparticle calculations

Y. Zhang, W. Xia, Y. Wu, and P. Zhang

1/1/2019

Significance of hydrogen bonding networks in the proton-coupled electron transfer reactions of photosystem II from a quantum-mechanics perspective

J. Chai, Z. Zheng, H. Pan, S. Zhang, K. V. Lakshmi, and Y. Sun

1/1/2019

The Middle Road Less Taken: Electronic-Structure-Inspired Design of Hybrid Photocatalytic Platforms for Solar Fuel Generation

J. Cho, A. Sheng, N. Suwandaratne, L. Wangoh, J. L. Andrews, P. Zhang, L. F. J. Piper, D. F. Watson, and S. Banerjee

12/13/2018

Quasiparticle electronic structure of honeycomb C ₃ N: from monolayer to bulk

Y. Wu, W. Xia, W. Gao, F. Jia, P. Zhang, and W. Ren

11/22/2018

Hole Extraction by Design in Photocatalytic Architectures Interfacing CdSe Quantum Dots with Topochemically Stabilized Tin Vanadium Oxide

J. L. Andrews, J. Cho, L. Wangoh, N. Suwandaratne, A. Sheng, S. Chauhan, K. Nieto, A. Mohr, K. J. Kadassery, M. R. Popeil, P. K. Thakur, M. Sfeir, D. C. Lacy, T. Lee, P. Zhang, D. F. Watson, L. F. J. Piper, and S. Banerjee

11/1/2018

Ligand-Directed Stabilization of Ternary Phases: Synthetic Control of Structural Dimensionality in Solution-Grown Cesium Lead Bromide Nanocrystals

J. Cho, and S. Banerjee

8/7/2018

Quasiparticle band structures of CuCl, CuBr, AgCl, and AgBr: The extreme case

W. Gao, W. Xia, Y. Wu, W. Ren, X. Gao, and P. Zhang

7/5/2018

Tuning the Deoxygenation of Bulk-Dissolved Oxygen in Copper

C. Li, P. Zhang, J. Wang, J. A. Boscoboinik, and G. Zhou

4/5/2018

Automated generation and ensemble-learned matching of X-ray absorption spectra

C. Zheng, K. Mathew, C. Chen, Y. Chen, H. Tang, A. Dozier, J. J. Kas, F. D. Vila, J. J. Rehr, L. F. J. Piper, K. A. Persson, and S. P. Ong

3/20/2018

Striping modulations and strain gradients within individual particles of a cathode material upon lithiation

L. R. De Jesus, P. Stein, J. L. Andrews, Y. Luo, B. Xu, and S. Banerjee

1/1/2018

Red phosphorus in its two-dimensional limit: novel clathrates with varying band gaps and superior chemical stabilities

Z. Zhu, P. Cui, X. Cai, M. Xia, Y. Jia, S. Zhang, and Z. Zhang

1/1/2018

Mitigating Cation Diffusion Limitations and Intercalation-Induced Framework Transitions in a 1D Tunnel-Structured Polymorph of V₂O₅

G. A. Horrocks, A. Parija, L. R. De Jesus, L. Wangoh, S. Sallis, Y. Luo, J. L. Andrews, J. Jude, C. Jaye, D. A. Fischer, D. Prendergast, L. F. J. Piper, and S. Banerjee

12/12/2017

Theoretical insights into the uranyl adsorption behavior on vanadium carbide MXene

Y. Zhang, Z. Zhou, J. Lan, C. Ge, Z. Chai, P. Zhang, and W. Shi

12/1/2017

Engineering the Near-Edge Electronic Structure of SnSe through Strains

Y. Wu, W. Xia, W. Gao, W. Ren, and P. Zhang

9/11/2017

Influence of ligand shell ordering on dimensional confinement of cesium lead bromide (CsPbBr₃) perovskite nanoplatelets

J. Cho, H. Jin, D. G. Sellers, D. F. Watson, D. H. Son, and S. Banerjee

1/1/2017

Programming Interfacial Energetic Offsets and Charge Transfer in β-Pb_0.33V₂O₅/Quantum-Dot Heterostructures: Tuning Valence-Band Edges to Overlap with Midgap States

K. E. Pelcher, C. C. Milleville, L. Wangoh, J. Cho, A. Sheng, S. Chauhan, M. Y. Sfeir, L. F. J. Piper, D. F. Watson, and S. Banerjee