Article
Chemistry, Multidisciplinary
Peiwei You, Chao Lian, Daqiang Chen, Jiyu Xu, Cui Zhang, Sheng Meng, Enge Wang
Summary: In this study, a polymeric semiconductor-graphitic carbon nitride was chosen as a prototype substrate to investigate light-driven photocatalytic water splitting. The research reveals the transport channel of photogenerated charge carriers at the interface, proposes a three-step photoreaction mechanism, and presents insights for further development of efficient water-splitting photocatalysts from a dynamic perspective.
Review
Chemistry, Multidisciplinary
Sen Lin, Hongwei Huang, Tianyi Ma, Yihe Zhang
Summary: This review systematically summarizes and introduces the research on photocatalytic O-2 evolution, covering principles, classical water oxidation photocatalysts, and strategies for activity improvement. It aims to provide timely guidance for future research on O-2 evolution.
Article
Multidisciplinary Sciences
Yan Yang, Xiaoyu Chu, Hong-Yu Zhang, Rui Zhang, Yu-Han Liu, Feng-Ming Zhang, Meng Lu, Zhao-Di Yang, Ya-Qian Lan
Summary: By systematically engineering N-sites, architecture, and morphology, the authors have successfully improved the water splitting activity of beta-ketoamine COFs.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Xiaodong Li, Tiangui Hu, Shan Lin, Zhanhong Ma, Junfei Wang, Lixia Zhao
Summary: Ordered nanoporous structures can be achieved through selective electrochemical etching, resulting in a 2.7 times increase in photocurrent for porous GaN compared to planar GaN. The enhanced photocatalytic performance is mainly due to the increased specific surface area and modulation of the electric fields of incident light in the porous structures.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Chemistry, Physical
Bipeng Wang, Weibin Chu, Alexandre Tkatchenko, Oleg Prezhdo
Summary: The study developed a methodology for nonadiabatic molecular dynamics that utilizes machine learning to reduce the expensive calculations of nonadiabatic couplings and excited state energies, resulting in significant computational savings and improved efficiency.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Hong Pang, Wei Zhou, Huilin Hu, Lequan Liu, Jinhua Ye, Defa Wang
Summary: In this study, high crystalline zigzag GaN nanowires were successfully synthesized and achieved efficient photocatalytic overall water splitting by constructing polar surface. Compared with non-polar nanowires, the zigzag nanowires showed enhanced H2 and O2 evolution in the presence of sacrificial reagents. This work suggests that constructing polar surface with spatially separated H2 and O2 evolution sites on one-dimensional nanomaterial could be a new crystal engineering strategy for efficient photocatalysts towards overall water splitting.
APPLIED CATALYSIS A-GENERAL
(2023)
Article
Mechanics
Qingying Feng, Ying Zhang, Hao Feng, Dong Liu, Qiang Li
Summary: Plasmon-mediated photocatalytic water splitting can efficiently harvest solar energy. Experimental studies have shown the benefits of hot spots in plasmonic nanoclusters for photocatalysis, but the interactions between different nanoclusters are difficult to observe experimentally. Theoretical studies have used a water molecule adsorbed on a single plasmonic nanocluster as a model. In this study, a representative model with a water molecule placed between two gold nanoclusters was computationally investigated. The results show that the plasmonic configurations can tune the hot electron transfer mode and enhance the water splitting rate. The distance between the water molecule and the gold nanoclusters also affects the charge transfer chain and the accumulation of hot electrons on the water molecule, leading to unexpected results.
Article
Chemistry, Physical
Hidehisa Hagiwara, Motonori Watanabe, Sun Kim, Kohei Higashi, Tatsumi Ishihara
Summary: The modification effect of acene dyes on the photocatalytic water splitting activity of Pt-loaded KTa(Zr)O-3 was studied. The results showed that TIPS-PEN was the most effective dye, increasing the hydrogen formation rate by 14 times. The fluorescence spectrum analysis revealed that the excitation energy of KTa(Zr)O-3 was transferred to the Pt cocatalyst through the TIPS-PEN moiety. The water splitting activity was improved by irradiating with both ultraviolet and visible light. Under visible light irradiation, no water splitting reaction occurred, indicating a Z-scheme-type water splitting reaction similar to the two-step photoexcitation mechanism in plant photosynthesis occurred on PtOx/TIPS-PEN/KTa(Zr)O-3.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Review
Chemistry, Applied
Dinghua Zhou, Ke Fan
Summary: This review discusses recent advances in studies on hematite photoanodes for water splitting, and summarizes strategies for improving hematite PEC performance by enhancing photon absorption efficiency, semiconductor bulk separation efficiency, and surface injection efficiency.
CHINESE JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Multidisciplinary
Hao Hong, Jiaxun Song, Xingchen Pan, Mingrui Luo, Richard Notzel
Summary: Cu2O microcrystals are electrodeposited on a GaN photoanode to enhance the efficiency of solar water splitting. The optimized Cu2O deposition amount improves the photocurrent density due to the built-in electric field and band offsets of the n-GaN/p-Cu2O heterostructure, facilitating the separation and transport of photogenerated charge carriers.
Article
Nanoscience & Nanotechnology
Qiqi Zhang, Xin Chen, Zhongshan Yang, Tao Yu, Lequan Liu, Jinhua Ye
Summary: Precisely tailoring the nitrogen defects is a promising approach for enhancing the photocatalytic efficiency of C3N4. In this study, two-coordinated-N vacancies are selectively introduced into the C3N4 framework through a facile Cl- modification method, and the concentration of defects can be easily controlled by varying the usage of Cl- during thermal polymerization. The optimal defective C3N4 exhibits superior hydrogen and oxygen evolution rates and the highest apparent quantum efficiency among reported single-component C3N4 photocatalysts for overall water splitting. The Cl- modification facilitates the introduction of two-coordinated-N vacancies and promotes charge carrier separation efficiency, leading to greatly enhanced photocatalytic efficiency.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Engineering, Environmental
Jing Tang, Xiaoyun Ma, Jiaxing He, Xiangyue Liu, Mingde Li
Summary: CdS/Pt/UiO-67 composites, synthesized by using hierarchically structured Zr-based UiO-67 as support to disperse CdS and Pt NPs, exhibit higher activity of hydrogen evolution than pure CdS under visible light irradiation. Femtosecond transient absorption spectra reveal the charge separation kinetics in CdS/Pt/UiO-67. This work provides a deeper understanding of the charge transfer between semiconductor and MOF materials.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2022)
Article
Chemistry, Multidisciplinary
Gedeng Wan, Lichang Yin, Xing Chen, Xiaoxiang Xu, Jie Huang, Chao Zhen, Huaze Zhu, Biaohong Huang, Weijin Hu, Zhaohui Ren, He Tian, Lianzhou Wang, Gang Liu, Hui-Ming Cheng
Summary: The role of oxygen vacancies in the photocatalytic behavior of PbTiO3 has been studied and found to be crucial. Oxygen vacancies on the negatively polarized facet act as active sites for water oxidation into O-2, while defect-free sites prefer H2O2 as the oxidation product. This research provides important guidance for the design of efficient ferroelectric photocatalysts and their water redox reaction pathways.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Dujuan Dai, Xizhuang Liang, Beibei Zhang, Yuanyuan Wang, Qian Wu, Xiaolei Bao, Zeyan Wang, Zhaoke Zheng, Hefeng Cheng, Ying Dai, Baibiao Huang, Peng Wang
Summary: Efficient visible light photocatalyst for overall water splitting is still a challenge. This work investigates the use of tetragonal zircon BiVO4 prepared by epitaxial growth on FTO substrate, achieving overall water splitting with improved hydrogen evolution activity and solar hydrogen conversion efficiency after loading cocatalysts.
Article
Chemistry, Physical
Kejian Lu, Fei Xue, Feng Liu, Mengfan Li, Wenlong Fu, Hao Peng, Chunyang Zhang, Jie Huang, Ze Gao, Hongwen Huang, Maochang Liu
Summary: In this study, atomic-scale N-doped NaTaO3@Ta3N5 core-shell cubes were prepared by nitridation of cubic NaTaO3. The core-shell heterojunctions exhibited efficient and stoichiometric evolution of H2 and O2 from photocatalytic overall water splitting, with a quantum efficiency of 2.18% at 550 nm. The successful performance was attributed to the thin Ta3N5 shell, increased lifetimes of the photogenerated charges, and the type-I band alignment that promoted smooth charge flow from N-NaTaO3 to Ta3N5. The efficiency was further improved to 6.28% by in situ deposition of a Rh@Cr2O3 core-shell cocatalyst.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Weibin Chu, Wissam A. Saidi, Jin Zhao, Oleg Prezhdo
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2020)
Article
Chemistry, Physical
Ran Shi, Andrey S. Vasenko, Run Long, Oleg Prezhdo
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2020)
Correction
Chemistry, Multidisciplinary
Qijing Zheng, Wissam A. Saidi, Yu Xie, Zhenggang Lan, Oleg V. Prezhdo, Hrvoje Petek, Jin Zhao
Article
Multidisciplinary Sciences
Ti Wang, Linrui Jin, Juanita Hidalgo, Weibin Chu, Jordan M. Snaider, Shibin Deng, Tong Zhu, Barry Lai, Oleg Prezhdo, Juan-Pablo Correa-Baena, Libai Huang
Article
Chemistry, Multidisciplinary
Ce Xu, Hui Wen Yong, Jinlu He, Run Long, Alisson R. Cadore, Ioannis Paradisanos, Anna K. Ott, Giancarlo Soavi, Sefaattin Tongay, Giulio Cerullo, Andrea C. Ferrari, Oleg Prezhdo, Zhi-Heng Loh
Summary: The study investigates the hot-electron transfer dynamics at the 1L MoS2/Au interface using TR-PEEM and atomic force microscopy, revealing an exponential decay of electron transfer rates with a decay coefficient of about 0.06 angstrom(-1). Ab initio simulations suggest that surface plasmon-like states mediate hot-electron transfer and explain its weak distance dependence.
Article
Physics, Applied
Ritabrata Sarkar, Md Habib, Sougata Pal, Oleg V. Prezhdo
Summary: The chalcogen atom plays a crucial role in the charge separation and recombination dynamics of supramolecular nanohybrids composed of carbon nanotubes and organic molecules. The insights gained from this study provide valuable guidelines for optimizing photovoltaic efficiency in modern nanoscale materials.
JOURNAL OF APPLIED PHYSICS
(2021)
Article
Chemistry, Physical
Carlos Mora Perez, Dibyajyoti Ghosh, Oleg Prezhdo, Sergei Tretiak, Amanda J. Neukirch
Summary: CsPbBr3 quantum dots have been suggested for their application as bright green LEDs, but their optical properties are not fully understood. This study analyzes the ground and excited states of CsPbBr3 clusters with vacancy defects, finding that Br vacancies should be avoided to maintain LED performance. Charged defects may still cause red-shifting and lower absorbance in CsPbBr3 QDs, affecting their LED performance.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Andrey A. Kistanov, Vladimir R. Nikitenko, Oleg Prezhdo
Summary: This study investigated seven kinds of point defects in a two-dimensional phosphorus carbide gamma allotrope, finding that these defects have a significant impact on the electronic structure of the material, with slightly higher formation energies compared to other materials.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Multidisciplinary
Guoqing Zhou, Gang Lu, Oleg Prezhdo
Summary: Auger-type energy exchange is crucial in nanomaterials due to strong carrier-carrier interactions. A new ab initio technique was developed to accurately model Auger scattering with nonadiabatic molecular dynamics, describing charge-charge and charge-phonon scattering in a nonperturbative manner. This technique successfully reproduced experimental processes, providing detailed insights into carrier dynamics in nanomaterials with strong carrier-carrier interactions.
Article
Chemistry, Multidisciplinary
Yucheng Xiong, Guoqing Zhou, Nien-Chu Lai, Xiaomeng Wang, Yi-Chun Lu, Oleg Prezhdo, Dongyan Xu
Summary: This research demonstrates switchable n-type and p-type electrical conduction in Bi2Se3 nanoribbons through a facile chemical approach, opening up new possibilities for the development of thermoelectric devices and offering significant implications in the fields of spintronics and quantum computing.
Article
Chemistry, Physical
Wei Li, Juan Zhan, Xiaorui Liu, Jianfeng Tang, Wan-Jian Yin, Oleg Prezhdo
Summary: The use of alkali metal ions for defect passivation in lead halide perovskites has been shown to eliminate trap states and extend charge carrier lifetimes, improving the performance of perovskite solar cells. Atomistic understanding of the various factors contributing to defect passivation guides the development of high-efficiency perovskite devices.
CHEMISTRY OF MATERIALS
(2021)
Article
Chemistry, Physical
Lili Zhang, Weibin Chu, Chuanyu Zhao, Qijing Zheng, Oleg Prezhdo, Jin Zhao
Summary: The dynamics of small polarons induced by photoexcitation in rutile TiO2 were investigated using ab initio nonadiabatic molecular dynamics simulation, revealing significant differences in polaron formation, migration, and quenching at different temperatures. At low temperature, the polaron is localized on a single Ti atom and quenches slowly, while at increased temperature, thermal phonon excitation stimulates polaron hopping and delocalization, leading to fast polaron quenching within 200 ps.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Multidisciplinary
Zilong Wang, Patrick Altmann, Christoph Gadermaier, Yating Yang, Wei Li, Lavinia Ghirardini, Chiara Trovatello, Marco Finazzi, Lamberto Duo, Michele Celebrano, Run Long, Deji Akinwande, Oleg Prezhdo, Giulio Cerullo, Stefano Dal Conte
Summary: Experimental and quantum dynamics simulations indicate that charge separation in MoSe2/WSe2 heterostructures is ultrafast and temperature-independent, while recombination accelerates significantly with temperature. Charge separation is temperature-independent due to its barrierless nature, involvement of dense acceptor states, and promotion by higher-frequency vibrations, while the strong temperature dependence of recombination arises from modulation of indirect-to-direct bandgap by low-frequency motions.
Article
Chemistry, Physical
Weibin Chu, Oleg Prezhdo
Summary: A highly efficient and accurate method for numerical evaluation of nonadiabatic coupling in the Kohn-Sham representation with PAW pseudopotentials has been developed. It provides a significant improvement in accuracy without additional cost, compared to the current technique, and is much faster. The method simplifies NA evaluation in the core region, is robust to variations in the MD time step, and helps to maintain phase consistency of coupling.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Nanoscience & Nanotechnology
John A. Tomko, Evan L. Runnerstrom, Yi-Siang Wang, Weibin Chu, Joshua R. Nolen, David H. Olson, Kyle P. Kelley, Angela Cleri, Josh Nordlander, Joshua D. Caldwell, Oleg V. Prezhdo, Jon-Paul Maria, Patrick E. Hopkins
Summary: An energy transduction mechanism across metal/semiconductor interfaces has been demonstrated through ultrafast infrared spectroscopy, relying on electron-electron energy transfer instead of charge transport. The study shows a novel mechanism where hot electrons in metal transfer their energy to free electrons in semiconductor without charge transfer, providing a unique means to modulate plasmonic interactions. These findings are supported by optical modeling and first-principle calculations, indicating the potential for improved plasmonic enhancement beyond traditional charge injection mechanisms.
NATURE NANOTECHNOLOGY
(2021)