Article
Chemistry, Physical
Halima Begum, Seunghun Jung
Summary: In this study, a defective Prussian-blue/graphene composite electrocatalyst was prepared and exhibited remarkable electrocatalytic water splitting performance and durability in alkaline media.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Chemistry, Physical
Shiqian Cao, Yanyu Liu, Tingting Bo, Ruixin Xu, Nan Mu, Wei Zhou
Summary: The research focuses on improving the catalytic activity for water splitting by adjusting the electronic structure of graphene. G-SO4 shows high activity for both the hydrogen evolution reaction and oxygen evolution reaction, and the catalytic activity of functionalized graphene is strongly influenced by interfacial charge transfer and the pz band center of carbon active sites. This work provides a new idea for predicting and designing potential carbon-based catalysts for overall water splitting.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Physical
Yining Zhang, Sha Li, Chao Sun, Xiaorou Cao, Xi Wang, Jiannian Yao
Summary: Designing catalyst for ammonia synthesis at mild conditions is a meaningful challenge. In this study, defective g-C3N4 nanosheet supported single-cluster ruthenium and iron catalysts were investigated. It was found that the Ru-3/N-v-g-C3N4 catalyst exhibited a much higher turnover frequency than Ru(0001) at industrial reaction conditions. The reaction on Ru-3/N-v-g-C3N4 occurred through both dissociative and alternative associative mechanisms, while on Fe-3/N-v-g-C3N4 catalyst, it solely proceeded through the dissociative pathway.
Article
Chemistry, Physical
Yining Zhang, Sha Li, Chao Sun, Xiaorou Cao, Xi Wang, Jiannian Yao
Summary: By investigating the performance of single-cluster catalyst Ru-3/N-v-g-C3N4 in ammonia synthesis, it is revealed that this catalyst has high catalytic activity under mild conditions and the reaction is controlled by dissociative and associative mechanisms. In comparison, the catalytic activity of Fe-3/N-v-g-C3N4 catalyst is lower and the reaction only occurs through the dissociative pathway.
Article
Chemistry, Physical
Mosab Jaser Banisalman, Min-Cheol Kim, Sang Soo Han
Summary: A comprehensive theoretical study on NH3 synthesis of bimetallic Ru-Co catalysts using density functional theory and microkinetic modeling has been conducted, revealing that the spin-symmetry breaking of RuCo surface enables more facile N-2 dissociation and enhances catalytic activity for NH3 synthesis, providing an alternative strategy to catalyst design.
Article
Nanoscience & Nanotechnology
Esmaeil Zaminpayma, Payman Nayebi, Mohsen Emami-Razavi
Summary: The transport properties and rectification behavior of junctions containing armchair graphene nanoribbons with double vacancy defects or nitrogen doping in three different sizes were studied. Results showed that the presence of double vacancy defects and nitrogen doping can alter the behavior of the devices, with significant rectification observed in the 9-atom size devices.
Article
Chemistry, Physical
Michael Rebarchik, Saurabh Bhandari, Thomas Kropp, Manos Mavrikakis
Summary: Using first-principles density functional theory calculations, a pH-dependent microkinetic model is developed to evaluate the performance of transition metal catalysts embedded in nitrogen-doped graphene for the oxygen evolution reaction. It is found that reaction pathways involving intermediates co-adsorbed on the metal site are preferred and lead to enhanced catalytic activity. These findings highlight the importance of investigating reaction pathways on graphene-based catalysts and other two-dimensional materials with metal active centers decorated by spectator intermediate species.
Article
Chemistry, Physical
Manos Mavrikakis, Saurabh Bhandari, Thomas Kropp, Michael Rebarchik
Summary: Using first-principles density functional theory calculations, we developed a pH-dependent microkinetic model to evaluate the performance of transition metal catalysts embedded in nitrogen-doped graphene for the oxygen evolution reaction. We found that reaction pathways involving intermediates co-adsorbed on the metal site are preferred and lead to enhanced catalytic activity compared to thermodynamics-based predictions. These findings highlight the importance of investigating reaction pathways on graphene-based catalysts and other two-dimensional materials involving metal active centers decorated by spectator intermediate species.
Article
Chemistry, Physical
Pilsun Yoo, Peilin Liao
Summary: We investigated the redox mechanisms of the water-gas shift reaction on the Fe3O4 (1 1 1) surface using DFT calculations and MKM. The reaction pathways involved three LH processes and one MK process. Both single and dual binding sites played a role in CO oxidation, with significant differences in activation energy and reaction rates observed among the four mechanisms.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Physical
Ojus Mohan, Shambhawi Shambhawi, Rong Xu, Alexei A. Lapkin, Samir H. Mushrif
Summary: A multiscale analysis combining density functional theory (DFT) and microkinetic modeling was conducted to resolve uncertainties in the CO2 methanation reaction mechanism on popular Ni and Ru catalysts. The study revealed that the dominant pathway on both Ni and Ru surfaces involves direct dissociation of CO2* to CO*.
Article
Multidisciplinary Sciences
Zhicheng Wu, Sifan Xu, Yong Zhou, Qilin Guo, Yuriy Dedkov, Elena Voloshina
Summary: This study presents a theoretical description of water molecule adsorption on NiPX3 surfaces, finding that physisorption occurs in all cases, while water dissociative adsorption is unfavorable. This work provides a foundation for further research on water/MPX3 reactions.
ADVANCED THEORY AND SIMULATIONS
(2021)
Article
Chemistry, Physical
Gagus Ketut Sunnardianto, George Bokas, Abdelrahman Hussein, Carey Walters, Othonas A. Moultos, Poulumi Dey
Summary: The study reveals that hydrogenated defective graphene structure, V-222, shows more reversible hydrogen adsorption and desorption processes compared to pristine graphene, providing a new pathway for improving hydrogen storage efficiency.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Chemistry, Multidisciplinary
Julia Bord, Bjoern Kirchhoff, Matthias Baldofski, Christoph Jung, Timo Jacob
Summary: Density functional theory (DFT) is utilized to investigate the electronic structure of platinum clusters on different graphene substrates. The size and defects of both the clusters and the graphene substrates are examined. The results reveal that larger vacancies lead to stronger binding of Pt clusters, while defect-free graphene shows more exothermic formation energy with increasing cluster size. Oxygen-free graphene supports are crucial for successful attachment of Pt, and cluster stability depends on the number and ratio of Pt-C, Pt-Pt, and Pt-O bonds rather than the cluster geometry.
Review
Chemistry, Physical
Yu Hao, Tian-Yu Sun, Liang-Feng Huang
Summary: This article reviews the role and microscopic mechanisms of defective MoS2 in electrochemical reactions from the perspective of density-functional-theory simulation. It also projects the future research trends and challenges in the electrochemical catalysis and corrosion of defective MoS2.
CURRENT OPINION IN ELECTROCHEMISTRY
(2022)
Article
Chemistry, Physical
Lang Xu, Eric E. Stangland, James A. Dumesic, Manos Mavrikakis
Summary: Catalytic hydrodechlorination of 1,2-dichloroethane using Pt catalysts was studied through a synergistic approach of DFT calculations, reaction kinetics experiments, and microkinetic modeling. The reaction on Pt(111) involves multiple steps leading to the formation of ethane. Adjustments to model parameters were made to achieve good agreement between theoretical predictions and experimental results, highlighting the importance of coverage effects in catalytic reactions. Overall, the study provides valuable mechanistic insights for improving catalysts in this chemistry.
Article
Chemistry, Physical
Qi Luo, Xiangyu Guo, Lihong Zhang, Shiping Huang
Summary: The structure and electronic properties of (PdH)(N) clusters were investigated using the artificial bee colony algorithm and DFT calculations. The clusters tend to have spherical disordered geometry, with hydrogen atoms mainly on the surface in two-fold bridge or three-fold hollow sites. Charge transfer from Pd to H atoms was observed, and the clusters exhibited non-magnetic or weakly magnetic characteristics.
THEORETICAL CHEMISTRY ACCOUNTS
(2021)
Article
Engineering, Environmental
Manman Ren, Xiangyu Guo, Shiping Huang
Summary: This study constructs a series of Fe single-atom catalysts coordinated by B atoms, and systematically investigates the electrocatalytic CO2 reduction reaction (CO2RR). FeB2C and FeB(2)C(2)h show higher CO2RR activity, with FeB2C exhibiting the best performance. This provides a new theoretical perspective for the rational design of high activity, selective CO2RR catalysts.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Physical
Yu Zou, Xiangyu Guo, Xiaoqiong Bian, Yongfan Zhang, Wei Lin, Shuping Huang, Zhongfang Chen, Kaining Ding
Summary: The production of hydrogen peroxide (H2O2) is important in human lives. However, designing efficient catalysts for the two-electron oxygen reduction reaction (2e- ORR) remains challenging. Inspired by superoxide dismutase, we designed eight types of 2e- ORR catalysts and found that NiN2S2/BN showed the most favorable catalytic performance. Our work also revealed the effects of coordination environment changes on oxygen adsorption behavior, electron density around Ni, and work function.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Physical
Xiaoqiong Bian, Yu Zou, Wenkai Chen, Wei Lin, Xiangyu Guo, Kaining Ding
Summary: Using density functional theory (DFT) calculations, this study explored the catalytic performance of four types of graphene-based single-atom catalysts (SACs) towards the electrochemical acetonitrile (CH3CN) reduction reaction. Two highly stable SACs, Cr@N4 and Mn@N4, were identified to greatly accelerate reaction thermodynamics and kinetics with small energy barriers. These SACs effectively suppress the competitive hydrogen evolution reaction (HER) and exhibit superior catalytic selectivity. The adsorption energy of *CH3CHN is directly correlated to the activity trends of various candidates, and the bonding/anti-bonding interactions between different active metal centers and *CH3CHN determine the adsorption strength. The study provides important theoretical guidance for constructing carbon-based materials supported transition metal single-atom electro-catalysts for the CH3CN reduction reaction.
APPLIED SURFACE SCIENCE
(2022)
Article
Physics, Multidisciplinary
Lei Zheng, Xiaojun Yang, Jian Li, Ruhui Yang, Hengze Qu, Xiangyu Guo, Shiping Huang, Shengli Zhang
Summary: This study provides a detailed comparison of the seven polymorphs of VOPO4 using density functional theory (DFT). The results show that six of them are indirect bandgap semiconductors, one is a direct bandgap semiconductor, and one is an insulator. These findings shed light on the potential applications of VOPO4.
Article
Chemistry, Physical
Jing Li, Xiangyu Guo, Xuemin Hu, Wei Wang, Yuanyuan Tai, Min Xie, Zhi Li, Shengli Zhang, Haibo Zeng
Summary: The interface engineering strategy proposed in this study utilizes the structural characteristics of perovskite and the mirror asymmetry of 2D Janus material to achieve multifunctionality in the CsPbBr3/Janus MoSSe heterostructure. By modulating the atomic terminal contacts, both type-I and type-II band alignment can be achieved simultaneously in this heterostructure. The interface dipole and its induced interface potential step play a crucial role in shifting the band alignment. The interface effect enables adjustable band gaps and band types, as well as improved light absorption in the visible and ultraviolet regions. Furthermore, gate voltage regulation can transition the band alignment from intrinsic type-II to type-I or type-III in the CsBr-T/SMoSe heterostructure. These findings expand the functionality of perovskite-based heterostructures and provide possibilities for high-efficiency multifunctional nanodevices.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Physical
Xiaoqiong Bian, Qianqian Liu, Shuyi Xie, Wenkai Chen, Xiangyu Guo, Kaining Ding
Summary: Through density functional theory calculations, it was found that the metalloid boron atom can act as a highly active site for the electrochemical reduction of acetonitrile. The boron doped catalysts, specifically B/C2N, demonstrated excellent stability, selectivity, and resistance to poisoning. The boron-embedded C2N (Bint/C2N) showed the highest catalytic performance with the lowest limiting potential of -0.11 V. This work provides theoretical guidance for the development of novel and efficient metal-free electrocatalysts for the reduction of acetonitrile.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Manman Ren, Xiangyu Guo, Shengli Zhang, Shiping Huang
Summary: Using density functional theory computations, researchers identified graphdiyne and holey graphyne supported single-atom catalysts (SACs) as promising candidates for electrochemical CO2 reduction reaction (CO2RR). They found 25 catalysts that effectively activate CO2 and inhibit hydrogen evolution, with 8 of them showing higher activity for CH4 production than Cu(211). The study also revealed the impact of support materials on limiting potentials and reaction pathways, and machine learning was used to predict the activity of other SACs.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Xinliang Fu, Mei Wang, Yuanzhi Jiang, Xiangyu Guo, Xin Zhao, Changjiu Sun, Li Zhang, Keyu Wei, Hsien-Yi Hsu, Mingjian Yuan
Summary: Mixed-halide perovskites can be precisely tuned across the entire spectral range using composition engineering. However, ion migration in mixed halide perovskites under continuous illumination or electric field hinders the application of perovskite light-emitting diodes (PeLEDs). A novel approach that introduces strong and homogeneous halogen bonds within the quasi-two-dimensional perovskite lattices effectively suppresses ion migration, enhancing the stability of quasi-2D mixed-halide perovskite films. These PeLEDs exhibit an impressive 18.3% EQE with pure red emission and demonstrate a long operational half-life of approximately 540 minutes, making them one of the most stable mixed-halide pure red PeLEDs reported to date.
Article
Chemistry, Multidisciplinary
Xiangyu Guo, Shengli Zhang, Liangzhi Kou, Chi-Yung Yam, Thomas Frauenheim, Zhongfang Chen, Shiping Huang
Summary: In this study, a data-driven framework was developed to explore potential 2D materials with high electrocatalytic activity and stability for oxygen electrocatalysis. Through comprehensive evaluation of over 6300 materials, 1411 candidates were identified, and further computational analysis revealed the possible dissolution and oxidation of active materials under reaction conditions. Based on these findings, 24 ORR catalysts and 2 OER catalysts with superior activity and stability were screened out, providing a pathway for designing high-performance electrocatalysts for practical applications.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Physical
Lihong Zhang, Xiangyu Guo, Shengli Zhang, Thomas Frauenheim, Shiping Huang
Summary: This study reports a new type of double atom catalysts (HDACs) for the hydrogen evolution reaction (HER). By introducing nonmetal atoms near the metal sites, unique charge communication is enabled, leading to different catalytic activity compared to single atom counterparts. Machine learning analysis identifies key characteristics affecting catalytic activity and establishes a predictable framework for fast screening of unknown HDACs.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Lili Xu, Lei Zheng, Yu Jing, Xiangyu Guo, Xuemin Hu, Bo Xu, Shengli Zhang
Summary: This study conducted high-throughput calculations to find new candidate materials for the electron transport layer of high-performance perovskite light-emitting diodes. Among the identified candidates, 2D Tp-DAAQ and 2D Tp-DABDA with electron-accepting substituents showed the most promising performance.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Lihong Zhang, Xiangyu Guo, Shengli Zhang, Shiping Huang
Summary: Efficiently designed atomically dispersed bi-atom catalysts show promising catalytic activity for hydrogen evolution, oxygen reduction, and oxygen reduction reactions, providing a new direction for developing renewable energies.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Materials Science, Multidisciplinary
Ning Han, Xiangyu Guo, Junling Cheng, Pengyun Liu, Shuguang Zhang, Shiping Huang, Matthew R. Rowles, Jan Fransaer, Shaomin Liu
Summary: Ruddlesden-Popper perovskite oxide membranes doped with Mo show improved ionic conductivity and crystal stability, inhibiting phase transitions and enhancing oxygen permeability. The membranes exhibit high oxygen flux, permeation stability, and CO2 tolerance, making them an effective method for oxygen separation.
Article
Chemistry, Multidisciplinary
Xiangyu Guo, Shiru Lin, Jinxing Gu, Shengli Zhang, Zhongfang Chen, Shiping Huang
Summary: The research shows that MBenes can serve as efficient pH-universal catalysts for ammonia production, demonstrating exceptional activity and selectivity, large active surface area, and antioxidation properties.
ADVANCED FUNCTIONAL MATERIALS
(2021)
