Article
Chemistry, Physical
Hongyan Zhao, Hao Cao, Zisheng Zhang, Yang-Gang Wang
Summary: In this study, a methodology of Langmuir adsorption model-derived potential-dependent kinetics (LPD-K) was developed to probe the potential-dependent kinetics of CO2 reduction reaction (CO2RR) on single-metal atom electrocatalysts. The reaction mechanisms and energetics at the electrochemical interface were investigated using ab initio molecular dynamics simulations, and the onset potentials of CO2RR were predicted based on the correlations of potential-dependent free energetics and the proposed kinetic model.
Article
Chemistry, Physical
Hao Cao, Zisheng Zhang, Jie-Wei Chen, Yang-Gang Wang
Summary: This study investigates the potential-dependent activity and selectivity for the CO2 reduction reaction (CO2RR) on a single-iron-atom catalyst. The results show that CO2 adsorption is coupled with electron transfer from the substrate and is dependent on the electrode potential. The study also reveals a linear scaling relationship between reaction free energy and potential for key elementary steps of CO2RR. This research provides insights into the solvation effect and emphasizes the importance of electrode potential in theoretical considerations of catalytic activity.
Article
Chemistry, Applied
Jiejie Li, Jian Liu, Bo Yang
Summary: The study reveals significant differences in the adsorption and desorption processes of CO2 and CO on Fe-N-Gra catalysts for CO2RR in an electrochemical environment compared to vacuum. These findings provide important insights for the design of efficient M-N-Gra-based CO2RR catalysts.
JOURNAL OF ENERGY CHEMISTRY
(2021)
Article
Chemistry, Physical
Ya-min Wang, Hui-Min Yan, Hao Cao, Jie-wei Chen, Hua Yang, Jia-yi Zhu, Juan Sun
Summary: This study investigates the interfacial structures on the Fe-N-4-C catalyst and the dynamic observation of the oxygen reduction reaction (ORR) using classic molecular dynamics (MD) and ab initio molecular dynamics (AIMD) simulations. The orientation and population of interfacial water are dependent on the potential. The study also reveals the formation of hydrogen bonds (H-bonds) and their evolution based on the potential. Furthermore, the research explores the relationship between reaction free energy/activation barrier and potential for key elementary ORR steps, providing insights into electrode potential's impact on electrochemical processes.
Article
Chemistry, Multidisciplinary
Long Lin, Haobo Li, Yi Wang, Hefei Li, Pengfei Wei, Bing Nan, Rui Si, Guoxiong Wang, Xinhe Bao
Summary: In this study, the temperature-dependent CO2 reduction reactions over Fe-N-C and Ni-N-C single-atom catalysts were investigated, revealing variations in selectivity and activity. The differences in CO Faradaic efficiency and current density between Fe-N-C and Ni-N-C catalysts at different temperatures were found to be attributed to the varied adsorption strength of key reaction intermediates during CO2RR.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Jing-Min Liu, Tomoki Nishigori, Toshihiko Maeyama, Qian-Rui Huang, Marusu Katada, Jer-Lai Kuo, Asuka Fujii
Summary: This study uses infrared photodissociation spectroscopy to investigate the ability of water to form hemibonds, providing firm evidence of water's hemibond formation capability.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Nicholas Winner, Haley Williams, Raluca O. Scarlat, Mark Asta
Summary: Understanding the solvation behavior of Cr in molten salts and its effect on coordination geometry, as well as the medium-range structure changes, is crucial for assessing the corrosivity of molten fluorides. The presence of Cr and its solvation within oligomer structures in different fluoride melts suggests that fluoroacidity alone may not be a sufficient metric for evaluating corrosion. The solvent-dependent manner in which Cr alters the medium-range structure highlights the importance of considering the short- and medium-range structure of the solvent in understanding its solvation behavior.
JOURNAL OF MOLECULAR LIQUIDS
(2021)
Review
Chemistry, Physical
Mohammad Hasibul Hasan, Ian T. McCrum
Summary: This article discusses the quantitative understanding of the effects of near-surface solvent on predictive catalyst and electrode design through the direct comparison between ab initio computational modeling and experimental measurements. It also provides a benchmark for different approximations and suggests improved modeling methodologies.
CURRENT OPINION IN ELECTROCHEMISTRY
(2022)
Article
Chemistry, Physical
Jia Zhao, Di Liu, Fenfei Wei, Weng Fai Ip, Hui Pan, Sen Lin
Summary: In this study, the influence of solvent molecules on CO2 reduction reaction (CO2RR) over single metal atom catalysts was systematically investigated. It was found that water molecules not only affect the electronic state of the metal atom, but also the energy and conformation of CO2RR intermediates, providing useful insights for the design of efficient CO2RR single atom catalysts.
Article
Chemistry, Physical
Hee-Joon Chun, Inkyung Kim, Juhun Park, Giwoong Ha
Summary: The interaction between conjugated polymers and BaTiO3 in different solvents was studied. The results showed that the degree of solvation through van der Waals forces and hydrogen bonding decreased with the increasing hydrophobicity of the solvents. In addition, the solvation interaction energy had a linear correlation with the experimental differential of zeta potential, indicating that the calculated energy was associated with the electrostatic environment at the dispersant/solvent/BaTiO3 interface.
APPLIED SURFACE SCIENCE
(2024)
Article
Chemistry, Physical
Lanlan Chen, Yanan Zhou, Yifei Rao, Mingxin Qin, Bingbing Gong, Wenhua Zhang, Zhenyu Li
Summary: Fe atom-decorated MoS2 has been found to be a stable and noble-metal-free catalyst for nitrogen reduction reaction (NRR) at ambient conditions. The synergetic effect between a single Fe atom and the directly bonded oxygen atoms in the Mo-edge of MoS2 is responsible for the high-performance of NRR, and moderate charge transfer between Fe and the support greatly promotes the NRR activity and selectivity.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Zhiqiang Bai, Wenhua Zhang, Yufang Liu
Summary: The potential application of 27 single atom catalysts (SACs) supported by N(O)-dual-doped graphene for the electroreduction of nitrogen is investigated. The results show that the ammonia selectivity can be improved by utilizing the reorganization of coordination environments under high coverage of reactant molecules. The electroreduction of nitrogen proceeds with high ammonia selectivity at low limiting-potential on certain SACs.
Article
Chemistry, Physical
Rafal Topolnicki, Przemyslaw Dopieralski
Summary: The study shows that in isolated benzene systems, deuterium atoms appear larger than protium atoms at higher temperatures, while hydrogen atoms have a larger volume at lower temperatures. Further research is needed on the isotope effect and inverse kinetic isotope effect, particularly in supporting one of the competing mechanisms of olfaction where molecular shape is crucial.
CHEMICAL PHYSICS LETTERS
(2021)
Article
Chemistry, Physical
Xian Yuan, Zhenhua Chen, Bin Huang, Yuping He, Naigen Zhou
Summary: The MoS2/M2CS2 heterostructures were found to be stable and exhibit metallic properties, with low diffusion barriers indicating excellent rate performances for various metal-ion batteries. The theoretical capacities for NIBs/LIBs were significantly higher than for KIBs/MIBs, demonstrating their suitability as anode materials. Additionally, the heterostructures showed promising potential for NIBs with lower open-circuit voltages and higher capacities compared to LIBs.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Materials Science, Multidisciplinary
Hongming Zhang, Ying Song, Yang Liu, Jiupeng Zhao, Yao Li
Summary: This study investigated the geometric structures and Na atom adsorption behaviors of vacancies, N, S, and NS codoped on graphene using first principles calculations. The results showed that NS-DV-G has appropriate formation energy, large adsorption energy, and lower Na atom migration energy barrier, making it a promising component for future electrode materials.
MATERIALS TODAY COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Zhen Yao, Guang-Jie Xia, Wei Cao, Ke-Han Zeng, Yang -Gang Wang
Summary: In this study, the selective hydrogenation mechanism of furfural on a copper surface in the aqueous phase was explored using density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations. The presence of water solvent had a significant effect on the reaction mechanism, along with the charge interactions between the reaction intermediates and the copper surface. A proton-shuttling mechanism was revealed, where the initial hydrogen source for reducing the carbonyl group in furfural came from the dissociation of adjacent water. The water solvation effect resulted in dynamic charge separation, reducing the energy barrier.
JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Physical
Imran Muhammad, Shehzad Ahmed, Hao Cao, Asif Mahmood, Yang-Gang Wang
Summary: The theoretical design of porous three-dimensional (3D) silicene structures with stable structures, high porosities, conductive natures, and high uptake of ions shows great potential as anode materials in lithium and calcium ion batteries.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Deng Wang, Jiabang Chen, Peide Zhu, Ying Qiao, Hang Hu, Jie Zeng, Jiyao Zhang, Geping Qu, Yanggang Wang, Xingzhu Wang, Alex K. -Y. Jen, Baomin Xu
Summary: Developing a facile method to prepare high-quality perovskite films without using the antisolvent technique is critical for upscaling the production of perovskite solar cells. By introducing pre-synthesized microcrystals as seed crystals, this study successfully promotes the formation of defect-free perovskite films, resulting in high-efficiency devices with enhanced stability. The best-performing device achieved a power conversion efficiency of 23.27% for small-area devices and 21.52% for large-area devices, which are among the highest reported efficiencies for antisolvent-free PVSCs.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Kun Wang, Guang-Jie Xia, Tianhui Liu, Yulong Yun, Wu Wang, Kecheng Cao, Fenfa Yao, Xin Zhao, Boyuan Yu, Yang-Gang Wang, Chuanhong Jin, Jiaqing He, Yan Li, Feng Yang
Summary: This study successfully synthesized ultrathin W2C and Mo2C nanowires confined in single-walled carbon nanotubes (SWCNTs) using a host-guest assembly strategy. The strong interaction between W/Mo and SWCNTs resulted in the anisotropic growth of carbide nanowires along a specific crystal direction, accompanied by lattice strain and electron donation to SWCNTs. The M2C@SWCNTs (M = W, Mo) catalysts constructed a delocalized and electron-enriched SWCNT surface, leading to highly selective semihydrogenation of alkynes.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Gang Wang, Xue-Lian Jiang, Ya-Fei Jiang, Yang-Gang Wang, Jun Li
Summary: Efficient CO2 hydrogenation into valuable products is a promising strategy for addressing environmental issues. This study proposes Fe-3 and Ru-3 cluster catalysts anchored on MoS2 substrates for highly selective CO2 hydrogenation. The electron structure analysis reveals different CO2 adsorption modes on Fe-3 andRu-3 clusters, leading to different hydrogenation pathways. Microkinetic simulations demonstrate highly selective reactivity for methanol and ethanol formation on Fe-3/MoS2 and Ru-3/MoS2, respectively. This work provides atomic-scale insights into CO2 transformation, guiding the design of selective catalysts for CO2 hydrogenation.
Article
Chemistry, Applied
Geping Qu, Deng Wang, Xiaoyuan Liu, Ying Qiao, Danish Khan, Yinxin Li, Jie Zeng, Pengfei Xie, Yintai Xu, Peide Zhu, Limin Huang, Yang-Gang Wang, Baomin Xu, Zong-Xiang Xu
Summary: Inorganic hole transport materials, especially NiOX, have shown great potential in enhancing the efficiency and stability of perovskite solar cells. However, the direct contact between NiOX and the absorbing layer poses challenges, leading to losses in photovoltage and fill factor. By using an ionic compound (QAPyBF4) as an additive, defects in the perovskite layer are passivated, improving carrier conduction and interactions with under-coordinated Ni cations. The decorated cells achieved a power conversion efficiency of 23.38% and a fill factor of 85.5% without complex surface treatments or NiOX doping.
JOURNAL OF ENERGY CHEMISTRY
(2023)
Article
Chemistry, Physical
Ying Qiao, Guang-Jie Xia, Wei Cao, Ke-Han Zeng, Qian-Li Guo, Xiao-Feng Yang, Ai-Qin Wang, Yang-Gang Wang
Summary: The selective activation of C-C bonds for converting cellulose biomass into valuable chemicals is a fundamental challenge. In this study, three potential active phases were modeled, and constrained molecular dynamics simulations revealed that low-coordinated W center can chelate with glucose to form a metallacyclic complex, leading to the selective cleavage of C-C bond to produce valuable ethylene glycol. The reduced W5+ center is suggested to play a crucial role in stabilizing the dissociated C4 intermediates.
JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Physical
Xin-Mao Lv, Hong-Yan Zhao, Yang-Gang Wang
Summary: In this work, a Continuous Constant Potential Model (CCPM) based on grand canonical density functional theory is proposed to describe the electrocatalytic thermodynamics on single atom electrocatalysts dispersed on graphene support. The model considers the net charge variation of the electrode surface and evaluates the free energetics using a linearly potential-dependent capacitance. The model is demonstrated using the CO2 electro-reduction reaction on single-copper atom catalysts dispersed by nitrogen-doped graphene to predict the potential-dependent free energetics. The study shows that the net charges of catalyst models are quadratically correlated with the applied potentials and the quantum capacitance is linearly dependent on the applied potentials. It also suggests that CO2 adsorption coupled with electron transfer is an energetically unfavorable step on the CuN4@Gra model, while hydrogen adsorption is easily favored, likely resulting in the reconstruction of the CuN4@Gra catalyst as observed in experiments. The CuN2@Gra model exhibits higher activity for CO2RR at the C site, and the potential determining step shifts to the *CO formation step at a wide potential range.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Weiming Chen, Zhen Yao, Wenxing Chen, Qikai Shen, Desheng Yuan, Chi Zhang, Yifeng Zhu, Hai-Wei Liang, Yang-Gang Wang, Weiguo Song, Changyan Cao
Summary: Fully exposed cluster catalysts (FECCs) with multiple metal atoms provide a bridge between single-atom catalysts (SACs) and nanoparticles (NPs). While FECCs have been extensively studied in dehydrogenation and oxidation reactions, their application in hydrogenation is limited. This study shows that fully exposed Ir clusters anchored on sulfur-doped carbon support exhibit higher activity and stability in the hydrogenation of N-heteroarenes compared to Ir SAC and Ir NPs catalysts. The reaction mechanism on Irn/SC is also elucidated.
Article
Chemistry, Physical
Tongxin Song, Zhen Yao, Guangjun Li, Xiao Cai, Xu Liu, Yang-Gang Wang, Weiping Ding, Yan Zhu
Summary: In this study, a heterodimeric gold cluster, Au-29(SR)(19), composed of two functional units fused by sharing four common Au atoms, is reported. One functional unit derived from the half structure of homodimeric Au(28)(SR)(20) cluster impacts catalytic reactivity, while the other functional unit composed of the half structure of homodimeric Au-30(SR)(18) cluster provides structural stability. The synergistic effect exhibited by this heterodimeric catalyst offers new insights into fundamental catalysis and the potential for improving catalytic properties.
Review
Chemistry, Multidisciplinary
Hongyan Zhao, Xinmao Lv, Yang-Gang Wang
Summary: The rational design of electrocatalysis is crucial for addressing energy and environmental crises. Understanding the complex electrochemical interface, including factors like electrode potential and H-bond network, is essential for optimizing electrocatalytic activity and selectivity. This review explores recent theoretical advances in modeling realistic electrocatalytic processes at complex interfaces and highlights the challenges and fundamental problems in this field. The significance of including explicit solvation and electrode potential, as well as strategies for designing highly efficient electrocatalysts, is discussed. The structure-activity relationships and dynamic responses of electrocatalysts to the environment are crucial for understanding complex interfaces and improving electrocatalytic activity.
Article
Chemistry, Multidisciplinary
Wei Cao, Guang-Jie Xia, Zhen Yao, Ke-Han Zeng, Ying Qiao, Yang-Gang Wang
Summary: Through DFT calculations and ab initio molecular dynamics simulations, the model reaction of formaldehyde hydrogenation with a Pt/TiO2 catalyst is studied with explicit solvent water molecules. In aqueous phase, both the O vacancy on support and solvent molecules could donate charges to a Pt cluster, with O vacancy dominantly reducing the Pt cluster from positive to negative. During the formaldehyde hydrogenation, the water molecules can protonate the O in the aldehyde group, generating the OH at the metal-support interface by long-range proton transfer. The presence of O vacancy on reduced support promotes the hydrogenation of OH, making it exergonic and kinetically more facile.
Article
Chemistry, Multidisciplinary
Imran Muhammad, Shehzad Ahmed, Zhen Yao, Danish Khan, Tanveer Hussain, Yang-Gang Wang
Summary: This study systematically investigates the potential of first-row two-dimensional transition metal carbides (TMCs) as sulfur cathodes for Li-S batteries, and finds that VC nanosheet possesses immense anchoring potential and exhibits a comparatively low migration energy barrier.
Article
Chemistry, Multidisciplinary
Imran Muhammad, Shehzad Ahmed, Hao Cao, Zhen Yao, Danish Khan, Asif Mahmood, Tanveer Hussain, Xiao-Gen Xiong, Rajeev Ahuja, Yang-Gang Wang
Summary: In this research, a porous material called sulfur-graphdiyne (3D-SGDY) was designed and a single copper atom was anchored in it, demonstrating its excellent performance in CO2 reduction and ion storage.
MATERIALS TODAY CHEMISTRY
(2023)
Article
Chemistry, Physical
Qilun Wang, Huawei Wang, Hao Cao, Ching-Wei Tung, Wei Liu, Sung-Fu Hung, Weijue Wang, Chun Zhu, Zihou Zhang, Weizheng Cai, Yaqi Cheng, Hua Bing Tao, Hao Ming Chen, Yang-Gang Wang, Yujing Li, Hong Bin Yang, Yanqiang Huang, Jun Li, Bin Liu
Summary: This study presents a catalyst composed of atomically dispersed iridium and phosphorus that acts as integrative catalytic pairs, boosting the performance for the hydrogen oxidation reaction. The catalyst exhibits superior performance in fuel cells compared to commercial platinum/carbon catalysts. This work not only advances the development of anodic catalysts for fuel cells, but also provides a precise and universal active-site design principle for multi-intermediate catalysis.