Article
Energy & Fuels
Lan Zhou, Dan Guevarra, John M. Gregoire
Summary: Metal oxide solar absorbers have great potential for solar energy conversion. By improving metal vanadates, such as iron and chromium vanadates, the conversion efficiency can be increased. Combinatorial synthesis and high throughput screening can improve the utilization of photons in specific energy ranges.
JOURNAL OF PHYSICS-ENERGY
(2022)
Article
Chemistry, Multidisciplinary
Maylis Orio, Dimitrios A. Pantazis
Summary: Quantum chemical approaches are a powerful tool in studying the properties and reactivity of metalloenzymes, particularly in the field of solar fuels research. These methods help in understanding the nature of catalytic intermediates, establishing structure-function correlations, elucidating functional principles, and unraveling key steps in reaction mechanisms.
CHEMICAL COMMUNICATIONS
(2021)
Review
Chemistry, Multidisciplinary
Jie Ouyang, Qi-Chao Lu, Sheng Shen, Shuang-Feng Yin
Summary: Converting and storing solar energy directly as chemical energy through photoelectrochemical devices are promising strategies to replace fossil fuels. Metal oxides face challenges such as limited light absorption, inefficient charge separation, sluggish surface reactions, and insufficient stability as photoanode materials. Regulation of surface oxygen species on metal oxide photoanodes has emerged as a critical strategy, but its precise role remains ambiguous. This review focuses on elucidating the formation and regulation mechanisms of surface oxygen species, their impact on photoelectrochemical reactions, and the characterization methods employed.
Article
Chemistry, Multidisciplinary
Lan Zhou, Yu Wang, Kevin Kan, Daphne M. Lucana, Dan Guevarra, Yungchieh Lai, John M. Gregoire
Summary: This study investigates ternary antimonate (X-Sb-O) materials as potential photoanodes for solar-driven water splitting to produce dioxygen. Through high-throughput methods and automated analysis, 19 photoanode phases with broad spectral response were discovered. The stability of ternary antimonates and the characteristics of main group oxides provide opportunities for the development of stable photoanodes in the future.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Nanoscience & Nanotechnology
Thanh Tai Nguyen, Malkeshkumar Patel, Sangho Kim, Vinh-Ai Dao, Joondong Kim
Summary: The implementation of transparent photoanodes using metal-oxide junctions has shown promising results in improving the efficiency of photoelectrochemical cells for solar-driven hydrogen generation. The study demonstrates the potential of stacked photoanodes with PTPE cells to enhance photocurrent, providing a pathway for the development of robust on-site energy generation systems.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Juan M. Coronado, Alicia Bayon
Summary: Solar thermochemical fuels are a promising low-carbon alternative to fossil fuels, with efficient conversion of solar to chemical energy. The use of solid oxygen carriers enables CO2 and H2O splitting, with the production of syngas. The connection between thermochemical cycles and catalysis requires exploration of their differences and similarities.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
C. Bhagya Lakshmi, S. Jeya Lakshmi, Jeyanthinath Mayandi, S. Anna Venus, R. Marnadu, X. Vasanth Winston, M. Aslam Manthrammel, Mohd. Shkir
Summary: CuBiSe/metal oxide (TiO2, V2O5, and ZnO) nanocomposites were synthesized using a simple and low-cost hydrothermal technique for Dye-Sensitised Solar Cells (DSSCs) application. Various analyses including XRD, XPS, SEM with EDX, FTIR, UV-Visible Spectroscopy, PL spectrum, Hall Effect analysis, and Impedance analysis were performed to evaluate the nanocomposites. The photovoltaic performance of DSSCs with CBS/TiO2, CBS/V2O5, and CBS/ZnO photoanodes was investigated. The CBS/V2O5 DSSCs device demonstrated a short-circuit photocurrent density of 3.728 mA cm2, an open circuit voltage of 0.398 V, a fill factor of 0.72, and a power conversion efficiency (PCE) of 1.07%, higher than that of DSSCs using CBS/TiO2 and CBS/ZnO photoanodes (PCE = 0.62 and 0.37%). These results suggest that the prepared nanocomposite is a suitable photoanodic material for DSSCs applications.
SURFACES AND INTERFACES
(2023)
Review
Biochemistry & Molecular Biology
Xuanzhen Li, Jing Xiong, Zhiling Tang, Wenjie He, Yingli Wang, Xiong Wang, Zhen Zhao, Yuechang Wei
Summary: This paper evaluates excellent photocatalysts based on TiO2, WO3, ZnO, Cu2O, and CeO2 metal oxide materials, which are cost-effective, long-lasting, and easy to fabricate. Strategies to improve CO2 conversion efficiency, such as heterojunction, ion doping, defects, sensitization, and morphology control, are summarized. The 3DOM material with a three-dimensional ordered macroporous structure is highlighted as an excellent candidate for CO2 conversion. Based on the discussion, new insights and prospects for designing high-efficient metallic oxide photocatalysts to reduce CO2 emissions are presented.
Article
Electrochemistry
H. Sameie, A. A. Sabbagh Alvani, B. T. Mei, R. Salimi, D. Poelman, F. Rosei
Summary: The Mo-doped ZnV2O6/rGO composite as a photoanode for photoelectrochemical (PEC) hydrogen production shows enhanced hole transfer efficiency and improved carrier separation and transfer. The synergistic enhancement in PEC performance, with a significant increase in incident photon-to-current efficiency, makes it a promising candidate for high-performance PEC visible-light-induced water-splitting devices.
ELECTROCHIMICA ACTA
(2021)
Article
Energy & Fuels
Siddharth Sradhasagar, Omkar Subhasish Khuntia, Srikanta Biswal, Sougat Purohit, Amritendu Roy
Summary: In this study, machine learning models were developed to predict the bandgap and its character of double perovskite materials, with LGBMRegressor and XGBClassifier models identified as the best predictors. These models were further employed to predict the bandgap of novel bismuth-based transition metal oxide double perovskites, showing high accuracy, especially in the range of 1.2-1.8 eV.
Article
Chemistry, Inorganic & Nuclear
Tanakorn Osotchan, Taweesak Sudyoadsuk, Surangkana Wannapop, Asanee Somdee
Summary: Metal ferrite oxides (MFe2O4) and iron oxide (Fe2O3) were investigated as unassisted operation for solar light harvesting photoelectrochemical cell (PEC). Different metal ferrite oxides, such as CuFe2O4, NiFe2O4, and ZnFe2O4, were synthesized using electrochemical deposition method. The crystal structure, surface morphology, and chemical composition of Fe2O3 and metal ferrite oxides were characterized using various techniques. CuFe2O4 showed p-type semiconductor characteristic, while Fe2O3, NiFe2O4, and ZnFe2O4 exhibited n-type semiconductor characteristic. Therefore, the coupling between n-type and p-type semiconductors can form PEC without external bias. CuFe2O4 was set as the photocathode, and the others were set as the photoanode. Both parallel and tandem configurations were explored. All materials can be used as unbiased PEC, and the best performance was observed with Fe2O3 coupled with CuFe2O4. The maximum photocurrent of Fe2O3-CuFe2O4 tandem PEC was around 6 mu A/cm(2) under parallel illumination conditions.
INORGANIC CHEMISTRY COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Hannah J. Sayre, Lei Tian, Minjung Son, Stephanie M. Hart, Xiao Liu, Daniela M. Arias-Rotondo, Barry P. Rand, Gabriela S. Schlau-Cohen, Gregory D. Scholes
Summary: Photocatalysis for organic synthesis has the potential to transform the chemical manufacturing industry, lower energy requirements, and operate at or near ambient conditions. However, a key challenge lies in delivering sufficient scale of photoenergy for efficient operation of the catalyst.
ENERGY & ENVIRONMENTAL SCIENCE
(2021)
Article
Nanoscience & Nanotechnology
Xiu-Shuang Xing, Xuyang Zeng, Zhongyuan Zhou, Zeinhom M. El-Bahy, Mohamed H. Helal, Qianyu Gao, Hassan Algadi, Peilin Song, Xuzhao Liu, Xinru Zhang, Jimin Du
Summary: This study presents a facile strategy to enhance the performance of photoelectrochemical water splitting using alpha-Fe2O3 photoanodes modified with metal-organic framework films doped with iron-group elements. The Co-doped MIL-125 catalyst exhibits the most excellent performance among the three dopants.
ADVANCED COMPOSITES AND HYBRID MATERIALS
(2023)
Review
Chemistry, Inorganic & Nuclear
Chizoba Ezugwu, Shengwei Liu, Chuanhao Li, Serge Zhuiykov, Soumyajit Roy, Francis Verpoort
Summary: Artificial photosynthesis is a promising technique for CO2 mitigation and solar energy conversion. Metal-organic frameworks (MOFs) are efficient photocatalysts with high surface area and flexible design capabilities for complex multicomponent systems. The review examines strategies for designing MOFs to convert CO2 into solar fuels efficiently, highlighting features as semiconductor photocatalysts and means to improve light-harvesting and CO2 adsorption.
COORDINATION CHEMISTRY REVIEWS
(2022)
Article
Chemistry, Physical
Abdussalam M. Elbanna, Kholoud E. Salem, Abdelrahman M. Mokhtar, Mohamed Ramadan, Mariam Elgamal, Hussein A. Motaweh, Hassan M. Tourk, Mohamed A-H Gepreel, Nageh K. Allam
Summary: By optimizing the alloy composition and fabrication process, we successfully prepared Ti-Mo-Fe alloy nanotubes with enhanced conductivity, improved photocatalytic performance, and remarkable stability. These optimized nanotubes showed better photocatalytic activity compared to bare TiO2 nanotubes.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Materials Science, Multidisciplinary
Julian Self, Nathan T. T. Hahn, Kristin A. A. Persson
Summary: We report the dielectric constant of 1 M LiPF6 in EC:EMC 3:7 w/w and neat EC:EMC 3:7 w/w. The EC solvent strongly coordinates with Li+ cations, leading to a loss of dielectric contribution. However, the identification of Li+ solvation shell is uncertain. The loss of free EC permittivity contribution is almost completely balanced by the positive contribution of LiPF6 salt.
ENERGY & ENVIRONMENTAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Caitlin A. McCandler, Jakob C. Dahl, Kristin A. Persson
Summary: Nanoclusters are promising materials due to their large surface areas and unique electronic structures. This study investigates the influence of ligands on the stability, bonding, and electronic structure of phosphine-stabilized gold nanoclusters. The addition of phosphine affects the morphology and functionality of the nanoclusters, highlighting the importance of considering the ligand environment.
Article
Nanoscience & Nanotechnology
Aditya Sood, Jonah B. Haber, Johan Carlstrom, Elizabeth A. Peterson, Elyse Barre, Johnathan D. Georgaras, Alexander H. M. Reid, Xiaozhe Shen, Marc E. Zajac, Emma C. Regan, Jie Yang, Takashi Taniguchi, Kenji Watanabe, Feng Wang, Xijie Wang, Jeffrey B. Neaton, Tony F. Heinz, Aaron M. Lindenberg, Felipe H. da Jornada, Archana Raja
Summary: In this study, lattice dynamics in photoexcited WSe2/WS2 heterostructures were directly visualized using femtosecond electron diffraction. It was found that both WSe2 and WS2 were heated simultaneously on a picosecond timescale, which cannot be explained by phonon transport across the interface. First-principles calculations revealed a fast channel involving layer-hybridized electronic states, enabling phonon-assisted interlayer transfer of photoexcited electrons. Phonons were emitted in both layers on the femtosecond timescale via this channel, consistent with the simultaneous lattice heating observed experimentally. Strong electron-phonon coupling via layer-hybridized electronic states was identified as a novel route for controlling energy transport across atomic junctions.
NATURE NANOTECHNOLOGY
(2023)
Article
Chemistry, Physical
Kang Yao, Na Li, Ning Li, Eric Sivonxay, Yaping Du, Kristin A. Persson, Dong Su, Wei Tong
Summary: Si-Sn thin film electrode shows excellent cycling stability, outperforming pure Si or Sn electrodes. Through first-principles calculations and in situ transmission electron microscopy studies, it is found that the Si-Sn electrode has reduced volume expansion, increased conductivity, and dynamic rearrangement upon lithiation. This work provides an important advance in understanding the lithiation mechanism of Si-based anodes for next-generation lithium-ion batteries.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Alexander Rizzolo Epstein, Evan Walter Clark Spotte-Smith, Maxwell C. C. Venetos, Oxana Andriuc, Kristin Aslaug Persson
Summary: Hydrolysis reactions are widely present in biological, environmental, and industrial chemistry. Density functional theory (DFT) is commonly used to study the kinetics and reaction mechanisms of hydrolysis processes. This study introduces a new data set, BH2O-36, and evaluates different DFAs for their performance in aqueous chemistry applications.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Maxwell C. Venetos, Mingjian Wen, Kristin A. Persson
Summary: The nuclear magnetic resonance (NMR) chemical shift tensor is a sensitive probe of atom's electronic and local structure. Machine learning has been applied to predict isotropic chemical shifts from structure in NMR, but often ignoring the full chemical shift tensor. This study uses an equivariant graph neural network (GNN) to predict full 29Si chemical shift tensors in silicate materials and achieves high accuracy.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Correction
Chemistry, Multidisciplinary
Alexander R. Epstein, Jeremy Demarteau, Brett A. Helms, Kristin A. Persson
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Alexander R. Epstein, Jeremy Demarteau, Brett A. Helms, Kristin A. Persson
Summary: The design of circular polymers is necessary due to the lack of efficient recycling methods for many commodity plastics. Polydiketoenamines (PDKs) stand out for their ability to undergo selective depolymerization in strong acid, allowing monomers to be recovered. The chemistry of the cross-linker, far from the reaction center, has been found to affect the depolymerization rate of PDKs, with a proximal amine in the cross-linker significantly accelerating the process.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Evan Walter Clark Spotte-Smith, Samuel M. Blau, Daniel Barter, Noel J. Leon, Nathan T. Hahn, Nikita S. Redkar, Kevin R. Zavadil, Chen Liao, Kristin A. Persson
Summary: In this study, we combine computational chemical reaction network (CRN) analysis based on density functional theory (DFT) and differential electrochemical mass spectroscopy (DEMS) to study gas evolution from a model Mg-ion battery electrolyte. The results reveal H(2)O, C2H4, and CH3OH as major decomposition products, which are explained by identifying elementary reaction mechanisms using DFT. This combined theoretical-experimental approach provides a means to effectively predict electrolyte decomposition products and pathways when initially unknown.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Letter
Chemistry, Physical
Jianli Cheng, Bin Ouyang, Kristin A. Persson
Summary: We propose a doping strategy to mitigate the O3-to-O1 phase transformation in LiNiO2, improving its cycling stability. The introduction of high-valence dopants with similar ionic radii to Ni3+ stabilizes the bulk structure of LiNiO2 at high charge. This study provides general guidance for the development of Ni-rich, Co-free cathodes for lithium-ion batteries.
ACS ENERGY LETTERS
(2023)
Article
Nanoscience & Nanotechnology
Ann Rutt, Dogancan Sari, Qian Chen, Jiyoon Kim, Gerbrand Ceder, Kristin A. Persson
Summary: With the increasing demand for sustainable energy storage solutions as fossil fuels are being replaced by renewable energy sources, there is ongoing research and development on multivalent batteries, particularly magnesium (Mg) batteries, in hopes of surpassing the performance of lithium-ion batteries. However, the limited energy density and transport properties of Mg cathodes pose critical challenges. This study evaluates ABO(4) zircon materials (A = Y, Eu and B = V, Cr) as potential Mg intercalation cathodes, showing promising Mg-ion transport properties and successful Mg-ion intercalation in synthesized zircon YVO4, EuVO4, and EuCrO4 materials. Among them, EuVO4 exhibits the best electrochemical performance with repeated reversible cycling. The unique structural motif of overlapping polyhedra along the diffusion pathway appears to play a key role in facilitating good Mg-ion mobility, providing a structural design metric for future Mg cathode development.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Jordan Burns, Kristin A. Persson
Summary: In this study, oxygen evolution energies were calculated for different facets of a rock-salt-structured cation-disordered Li-excess, Mn-rich Li-ion cathode Li2MnO2F at different lithiation states. The results showed that Li2MnO2F is more resistant to oxygen loss compared to nonfluorinated counterparts, particularly the {110} and {112} facets. For the {100} facet, higher proportions of Li in an O coordination shell lead to lower oxygen evolution energy (E-O(similar to)) and facilitate oxygen loss. Surface fluorine has a weaker effect on increasing E-O(similar to) at higher lithiation states. Weak bonding interactions between Li and O were found to be associated with lower E-O(similar to) and a higher propensity for surface oxygen loss.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Qian Chen, Dogancan Sari, Ann Rutt, Jiyoon Kim, Gerbrand Ceder, Kristin A. Persson
Summary: As concerns about cost, resource availability, and safety of Li-ion batteries increase, energy storage solutions based on Na, Mg, Ca, and Zn have gained attention. In this study, zircon-type YPO4 was found to have a unique structural environment that enables superior conduction of multiple ions. A composition of Na0.0625YSi0.0625P0.9375O4 exhibited good Na(+) conductivity of 0.99 mS/cm at 300 K with an activation energy of 220 meV.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Michael J. Statt, Brian A. Rohr, Kris Brown, Dan Guevarra, Jens Hummelshoj, Linda Hung, Abraham Anapolsky, John M. Gregoire, Santosh K. Suram
Summary: This manuscript presents an event-sourced architecture for materials provenance (ESAMP) that addresses the challenges in data generation, ingestion, and materials state-aware machine learning in the field of accelerating materials discovery. By using this architecture, the evolution of a material's state can be tracked, leading to the generation of enhanced datasets for data-driven materials discovery.
Article
Chemistry, Multidisciplinary
Dan Guevarra, Kevin Kan, Yungchieh Lai, Ryan J. R. Jones, Lan Zhou, Phillip Donnelly, Matthias Richter, Helge S. Stein, John M. Gregoire
Summary: Advancements in artificial intelligence are expanding the automation of materials and chemistry experiments. The introduction of hierarchical decision-making has also motivated coordination among multiple research workflows. Researchers have developed HELAO-async, a framework for hierarchical experimental laboratory automation and orchestration using asynchronous programming, which enables coordinated workflows of adaptive experiments in materials acceleration platforms.