Article
Chemistry, Inorganic & Nuclear
Luana-Flavia Radu, Amr A. A. Attia, Radu Silaghi-Dumitrescu, Alexandru Lupan, R. Bruce King
Summary: The structures and energetics of binuclear ethylenedithiolate iron carbonyls with different numbers of carbonyl groups were studied using density functional theory. The lowest energy structures were predicted for each compound, with stability evaluations based on the dissociation of CO molecules.
INORGANICA CHIMICA ACTA
(2021)
Article
Chemistry, Inorganic & Nuclear
Cosmin Balaiu, Amr A. A. Attia, Alexandru Lupan, R. Bruce King
Summary: The series of vegi(R) dicarbenes synthesized by Kunz and co-workers provide rigid chelating bidentate ligands with carbon donor atoms. Density functional theory has been used to investigate the structures and energetics of the iron carbonyl complexes involving these ligands, revealing their potential in replacing carbonyl groups and interacting with metal atoms.
INORGANICA CHIMICA ACTA
(2021)
Article
Chemistry, Physical
Henry I. Eya, Nelson Y. Dzade
Summary: Chalcogenide perovskites have emerged as promising alternatives to conventional hybrid organic-inorganic halide perovskites due to their thermal and chemical stability. In this study, we used density functional theory to characterize the properties of BaZrS3, one of the most promising chalcogenide perovskites. We found that BaZrS3 has desirable characteristics for efficient photovoltaic applications, including a direct bandgap, high absorption coefficient, low reflectivity, and low refractive index.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Yangyang Li, Zhiqiang Rao, Zhisong Liu, Junming Zeng, Wentao Bao, Zijun Wang, Jiangbing Li, Feng Yu, Bin Dai, Ying Zhou
Summary: In this study, Ni catalysts supported by TiO2 nanoparticles were fabricated and showed significantly improved methane conversion of CO and CO2 at low temperatures under light irradiation. The photoinduced charge carriers on the surfaces of the Ni/TiO2 nanoparticles enhanced the formation of intermediate species in the methanation process, as well as the formation of CO2 delta- species conducive to CO2 activation in the CO2 methanation process.
Article
Chemistry, Multidisciplinary
Sounak Sarkar, Thomas Bjorn Egede Gronbech, Aref Mamakhel, Martin Bondesgaard, Kunihisa Sugimoto, Eiji Nishibori, Bo Brummerstedt Iversen
Summary: This study reports on the electron density analysis and Raman spectroscopy of two metal-organic frameworks, revealing the important role of metal-ligand bonds and imidazolate bonds in controlling the melting and decomposition processes of ZIF compounds.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
X. Xiao, X. Wang, C. Liu, Y. Li, G. Sun, Y. Han
Summary: This paper introduces a photocatalyst MMT@Cu2+-Fe3O4/TiO2 with functional bipartite hetero-interfaces, which improves the technical bottleneck of low visible light utilization and high carrier recombination efficiency of traditional TiO2. The study shows that this catalyst is beneficial for Rh-B degradation and Cr(VI) reduction under visible irradiation, and the treatment efficiency of mixed wastewater can reach up to 97%.
MATERIALS TODAY CHEMISTRY
(2023)
Article
Chemistry, Physical
Mingfang Zhang, Qingjie Feng, Sheng Li, Guangjun Nan
Summary: This study investigates the light-triggered charge transfer across TiO2/MAPbI(3) interfaces using density functional theory (DFT) and time-dependent DFT approach. The study reveals that the electrostatic interactions between the ends of MA cations and the photogenerated electrons can enhance or weaken the charge transfer across the interfaces. Additionally, positively charged iodine vacancies at the interfaces tend to inhibit the light-induced charge transfer. The dipolar MA cations might have a dual effect on the hysteresis in PSCs with TiO2/MAPbI(3) interfaces.
Article
Nanoscience & Nanotechnology
Paolo Restuccia, Gabriele Losi, Omar Chehaimi, Margherita Marsili, M. Clelia Righi
Summary: Adhesion energy, a crucial quantity in various fields, determines the mechanical behavior and failure of interfaces. However, there is a lack of systematic and accurate first-principles determination of heterostructure adhesion energy due to the difficulties in simulating systems with different lattices. In this study, we have developed a robust workflow to search for optimal interface geometry and accurately determine adhesion energies for metallic heterostructures, creating a database of accurate values for technological applications. This allows us to benchmark empirical relations and improve their predictability using easily measurable or computable quantities.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Nanoscience & Nanotechnology
Chihiro Iwamoto, Yoshimi Ohtani, Kensuke Hamada
Summary: In-situ transmission electron microscopy (TEM) was used to investigate the microstructure evolution during ultrasonic bonding. It was observed that numerous nanoparticles were generated and moved randomly between the contact regions of the aluminum sheets. These nanoparticles filled the gaps between the joining partners, facilitating the formation of the bonded interface. The in-situ TEM observation technique provides a new approach to study ultrasonic bonding process.
SCRIPTA MATERIALIA
(2023)
Article
Chemistry, Multidisciplinary
Enrique Montes, Hector Vazquez
Summary: Using density functional theory (DFT), the electronic and conducting properties of benzenediamine connected to gold electrodes via different tip structures were investigated. Different binding motifs and junction spectral properties were examined, with corrections to molecular resonances at the junction based on atomistic structure of the tip. DFT-based transmission spectra approximated by a Lorentzian model involving only the highest occupied molecular orbital (HOMO) can achieve conductance values in quantitative agreement with previous experiments.
APPLIED SCIENCES-BASEL
(2021)
Article
Materials Science, Multidisciplinary
G. Kruthika, P. Ravindran
Summary: In this study, the interface between the solar cell absorber layer and electron transport layer was investigated using density functional calculations. It was found that there is a staggered band alignment between TiO2 and Cs2TiBr6, with Cs2TiBr6 showing higher absorption coefficient in the visible spectral region.
MATERIALS TODAY COMMUNICATIONS
(2022)
Article
Chemistry, Physical
D. Gemeri, J. C. Tremblay, M. Pastore, H. Bahmann
Summary: In this work, theoretical investigations of dye-sensitized solar cells using linear response time-dependent density functional theory (LR-TDDFT) and electron dynamics within the hybrid TDDFT/configuration interaction methodology are presented. The potential of local hybrid density functionals for these hybrid systems is evaluated through the study of electronic properties and energetic alignments of organic dyes on a typical semiconductor substrate. The accuracy of charge transfer excited states and the hybridization between interfacial states depend on the used exchange correlation functional. Furthermore, laser-induced charge migration dynamics shed light on the effect of hybridization on population transfer dynamics and charge injection rate.
Article
Chemistry, Physical
Xuehua Zhou, Juansu Zhang, Guoliang Bai, Chunhua Wang, Wenxiang He, Xiangnan Sun, Jianli Zhang, Jiaojiao Miao
Summary: Improving the charge transport characteristics is crucial for achieving the multifunction of molecule-based devices. Accurate measurement of the energy levels of molecular semiconductors is essential for evaluating their availability and optimizing device performance. A three-terminal hot electron transistor has been developed, which records the charge transport and provides in-situ characterization of the energy information as intrinsic properties of the molecular semiconductor.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Energy & Fuels
Agustin Baron Jaimes, Oscar Andres Jaramillo-Quintero, Ramses Alejandro Miranda Gamboa, Ariosto Medina-Flores, Marina Elizabeth Rincon
Summary: The ZnO/TiO2 bilayer ETM demonstrates the highest photovoltaic performance for Sb2S3 planar solar cells, achieving a champion efficiency of 5.08% with an open-circuit voltage of 0.58 V and a current density of 16.17 mA cm(-2). The use of ZnO/TiO2 promotes charge injection, decreases series resistance, and reduces charge recombination at the ETM/Sb2S3 interface.
Article
Chemistry, Physical
Diptarka Hait, Yu Hsuan Liang, Martin Head-Gordon
Summary: This study explores the prediction of molecular multipole moments and the assessment of performance in describing molecular interactions with external electric fields within density functional theory. The use of translationally invariant second cumulants matrix shows better performance, while some modern functionals may exhibit disappointing results.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
Cuncai Lv, Xianhua Bai, Shangbo Ning, Chenxi Song, Qingqing Guan, Bang Liu, Yaguang Li, Jinhua Ye
Summary: Converting CO2 into fuels or chemicals through photothermal catalysis is a promising solution for energy shortage and global warming. Understanding nanomaterial strategies in this process is crucial for device and catalyst design, as well as maximizing CO2 hydrogenation performance. This Perspective discusses nanomaterial design concepts, reviews recent progress, and highlights challenges and opportunities in photothermal CO2 hydrogenation.
Article
Chemistry, Physical
Yu Nie, Tingting Bo, Wei Zhou, Huilin Hu, Xiang Huang, Huaiyuan Wang, Xin Tan, Lequan Liu, Jinhua Ye, Tao Yu
Summary: Regulating the energy barrier of *COOH is crucial for the rate determining step in the photocatalytic reduction of CO2 to produce CO gas. In this study, an appropriate Zn vacancy on ZnIn2S4 was synthesized to enhance the photocatalytic CO2 reduction capacity (CO: 5.63 mmol g(-1) h(-1)) and selectivity (CO: 97.9%). Different sulfhydryl groups were used to regulate the formation of Zn vacancies in ZnIn2S4, leading to the generation of unsaturated sulfur coordination state adjacent to the Zn vacancy with fewer electrons compared to ZnIn2S4 without Zn vacancy. Experimental analysis and theoretical calculations demonstrated that the appropriate Zn vacancy shifted the Gibbs free energy of *COOH from endothermic to exothermic during the photoreduction of CO2. This work provides an engineering method to optimize cation vacancies and improve the efficiency of photocatalytic CO2 reduction by adjusting the energy barrier of intermediates.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Nanoscience & Nanotechnology
Zengming Man, Peng Li, Shuaishuai Liu, Yuman Zhang, Xiaolin Zhu, Siyuan Ye, Wangyang Lu, Wei Chen, Guan Wu, Ningzhong Bao
Summary: Graphdiyne (GDY) has achieved significant advancements in lithium-ion batteries (LIBs) due to its unique structure. The development of three-dimensional porous hydrogen-substituted GDY (HsGDY) with a large specific surface area, hierarchical porous structure, and expanded interlayer space has shown high-performance Li-ion storage capabilities. The HsGDY exhibits a large reversible capacity, superior cycle and rate performances, and fast Li-ion transport kinetics.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Nanoscience & Nanotechnology
Wuqing Luo, An Li, Baopeng Yang, Hong Pang, Junwei Fu, Gen Chen, Min Liu, Xiaohe Liu, Renzhi Ma, Jinhua Ye, Ning Zhang
Summary: A hexagonal phase ZnS photocatalyst is synthesized and exhibits higher CO selectivity and better activity for CO2 reduction reactions compared to cubic ZnS. The study provides valuable insights into the synthesis and electronic structure of hexagonal ZnS for CO2 reduction reactions, which can inspire the design of highly active photocatalysts.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Zhenjie Zhou, Peng Li, Zengming Man, Xiaolin Zhu, Siyuan Ye, Wangyang Lu, Guan Wu, Wenxing Chen
Summary: In this study, high-performance fiber-shaped supercapacitors (FSCs) based on a hybrid of nitrogen-doped carbon dots-Ti3C2Tx/silk nanofibers (NCDs-Ti3C2Tx/SNFs) were developed using microfluidic fabrication. The NCDs-Ti3C2Tx/SNFs possessed high volumetric capacitance, reversible charge-discharge stability, high energy density, good capacitance, and long-life cycles. The solid-state FSCs demonstrated practical energy-supply applications such as powering a lamp, watch, and toy car.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Xuelian Yu, Jian Xu, Jiangpeng Wang, Jinyu Qiu, Xiaoqiang An, Zhuan Wang, Guocheng Lv, Libing Liao, Jinhua Ye
Summary: In this study, a new protocol of natural Z-Scheme heterostructures based on red mud bauxite waste was demonstrated. The improved component and interfacial structure enabled efficient spatial separation of photo-generated carriers for overall water splitting, making it a promising photocatalyst for solar fuel production. This work presents the first Z-Scheme heterojunction based on natural minerals and provides a new avenue for the utilization of natural minerals for advanced catalysis applications.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Kang Peng, Jingying Ye, Hongjie Wang, Hui Song, Bowen Deng, Shuang Song, Yihan Wang, Linjie Zuo, Jinhua Ye
Summary: This study demonstrates that Ru nanoparticles supported on natural halloysite nanotubes can enhance the photothermal catalytic activity and selectivity of CO2 methanation under continuous flow conditions. The optimized catalyst exhibits a photothermal catalytic performance of 1704 mmolCH(4) g(cat)(-1) h(-1) with 93% CH4 selectivity and 68% CO2 conversion, surpassing other Ru-based catalysts in photothermal CO2 reduction. The excellent catalytic performance is attributed to the unique mesoporous tubular structure, efficient light-to-heat conversion, and interfacial interactions between halloysite nanotubes and Ru. This method of utilizing natural minerals as support provides a convenient approach for the rational design of abundant and low-cost catalysts for efficient photothermal catalytic CO2 reduction.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Xinmin Yang, Jiwei Cui, Xiaolu Liu, Qiqi Zhang, Defa Wang, Jinhua Ye, Lequan Liu
Summary: Cocatalyst is crucial in photocatalytic overall water splitting (POWS), but it also promotes H2-O2 recombination. In this study, a strategic approach of selectively coating single-layer graphene on metal cocatalyst was developed to suppress the backward reaction for efficient POWS. The results demonstrate the effectiveness of this method and its potential in developing cocatalysts with suppressed backward reaction for efficient POWS.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Bowen Deng, Hui Song, Qi Wang, Jianan Hong, Shuang Song, Yanwei Zhang, Kang Peng, Hongwei Zhang, Tetsuya Kako, Jinhua Ye
Summary: A Ru/In2O3 catalyst is reported for efficient and stable photothermal CH3OH production from CO2 hydrogenation under atmospheric pressure. The catalyst demonstrates a remarkable solar CH3OH production, which is more than 50 times higher than that of pure In2O3 and surpasses other reported In2O3-based photothermal catalysts. Detailed characterizations show that the interaction between Ru and In2O3 enhances the activation of CO2 and H-2, and Ru modulates the electronic structure of In2O3, promoting the generation of oxygen vacancies for CH3OH formation. This work provides a rational design approach for efficient catalysts in solar CH3OH production from CO2 hydrogenation under mild conditions.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Multidisciplinary Sciences
Yaguang Li, Xianhua Bai, Dachao Yuan, Chenyang Yu, Xingyuan San, Yunna Guo, Liqiang Zhang, Jinhua Ye
Summary: Cu-based high-entropy two-dimensional oxide is synthesized using a PVP templated method and shows enhanced sintering resistance and CO2 hydrogenation activity. It achieves a record photochemical energy conversion efficiency in photothermal CO2 hydrogenation under ambient sunlight irradiation.
NATURE COMMUNICATIONS
(2023)
Article
Multidisciplinary Sciences
Xin Chen, Junxiang Chen, Huayu Chen, Qiqi Zhang, Jiaxuan Li, Jiwei Cui, Yanhui Sun, Defa Wang, Jinhua Ye, Lequan Liu
Summary: In this study, a strategy of promoting water dissociation on Bi2O2CO3 is reported to achieve high solar to formate energy conversion in CO2 electroreduction. The authors identify CO3* as the key surface species for formate formation through electron spin resonance measurements and in situ Raman spectroscopy combined with isotopic labelling. The efficiency of solar to formate energy conversion reaches as high as 13.3% when combined with a photovoltaic device.
NATURE COMMUNICATIONS
(2023)
Review
Chemistry, Multidisciplinary
Bin Chang, Hong Pang, Fazal Raziq, Sibo Wang, Kuo-Wei Huang, Jinhua Ye, Huabin Zhang
Summary: In this review, the recent progress and challenges in preparing C2+ products are discussed. The recent advancements in carbon-carbon coupling results and proposed mechanisms are elaborated, along with the complex scenarios involved in the initial CO2 activation process, catalyst micro/nanostructure design, and mass transfer conditions optimization. The synergistic realization of high C2+ product selectivity through catalyst design and the influence of electrolytes using theoretical calculation analysis and machine learning prediction are also proposed. The in situ/operando techniques for tracking structural evolution and recording reaction intermediates during electrocatalysis are elaborated, as well as insights into triphasic interfacial reaction systems with improved C2+ selectivity.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Physical
Shuaishuai Liu, Yuchen Mao, Zhiyuan Su, Fan Fang, Kun Li, Yuhan Wu, Puyu Liu, Peng Li, Kun Chang
Summary: The construction of ZnIn2S4/ZnS (ZIS/ZnS) heterojunctions through a one-step solvothermal method greatly enhances the photocatalytic activity of the catalyst. The optimized ZIS/ZnS catalyst exhibits a significantly higher hydrogen evolution rate compared to pure ZnS and ZIS. The ZIS/ZnS heterojunction has high charge separation efficiency and a strong redox ability, and a Z-scheme electron transfer mechanism is proposed to explain the increased photocatalytic activity.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Chengcheng Zhang, Yingkui Yan, Hubiao Huang, Xinsheng Peng, Hui Song, Jinhua Ye, Li Shi
Summary: Fe@PCN-222 is an efficient and selective photocatalyst that can oxidize CH4 to liquid oxygenates at room temperature using visible light. The presence of Fe single-atoms promotes the transfer of photogenerated electrons and activates H2O2, resulting in a substantial improvement in the selectivity and activity of liquid oxygenate production.
Review
Chemistry, Physical
Long Yang, Amol U. Pawar, Ramesh Poonchi Sivasankaran, Donkeun Lee, Jinhua Ye, Yujie Xiong, Zhigang Zou, Yong Zhou, Young Soo Kang
Summary: This review focuses on the identification, conversion, reaction kinetics, pathways, and mechanisms of intermediates, as well as the efficiency and selectivity of multicarbon product formations during photocatalytic and electrocatalytic CO2 reduction. Theoretical simulations and calculations provide deeper insights into this process. Future research directions and inspirations are also included to guide the integration of catalytic systems.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
