Article
Chemistry, Physical
Yuqi Miao, Huashan Yan, Xianhui Qiu, Xiaowen Zhou, Dongmei Zhu, Xiaobo Li, Tingsheng Qiu
Summary: This study investigated the adsorption behavior of hydrated aluminum ions (Al3+) on kaolinite surface using density functional theory and molecular dynamics simulation. The results showed that hydrated aluminum ions preferentially form stable bidentate adsorption complexes on the kaolinite surface, and the Al-Os bond exhibits strong ionicity and bond filling characteristics.
APPLIED CLAY SCIENCE
(2022)
Article
Chemistry, Physical
Zilong Zhao, Kaiyu Wang, Guoyuan Wu, Dengbang Jiang, Yaozhong Lan
Summary: The adsorption behavior of Sc on the surface of kaolinite (001) was studied using density functional theory. Hydrated Sc3+, ScOH2+, and ScOH2+ species had coordination numbers of eight, six, and five, respectively. The adsorption model was based on ScOH2H2O5+, which had the most stable ionic configuration in the liquid phase. Adsorption of Sc ionic species was categorized into outer layer and inner layer adsorptions based on adsorption energy and bonding mechanism. Hydrated Sc ions were mainly adsorbed on the outer layer of the kaolinite (001)Al-OH and (00-1)Si-O surfaces through hydrogen bonding, while also being adsorbed on the inner layer of the deprotonated kaolinite (001)Al-OH surface through coordination bonding.
Article
Chemistry, Physical
Hongping Zhang, Meng Chen, Chenghua Sun, Youhong Tang, Yuxiang Ni, Faqin Dong
Summary: In this study, the interactions between mica and soil organic matters (SOMs) were investigated using density functional theory (DFT) calculations. The adsorption behavior of 12 typical SOMs on different types of mica (Na, K, or Cs) was systematically studied, and the details of the interactions were explored. The study found that the electronegativity and ionic radius of the cations in the mica were the most important factors in the interactions, followed by the configurations and functional groups of the SOMs. This work provides a detailed DFT-based method for understanding the effects of SOMs on mineral morphogenetic transformation.
APPLIED CLAY SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Seema Gautam, Neetu Goel
Summary: This study investigates the sensitivity of molybdenum phosphide (MoP) surfaces for CO2 activation using density functional calculations. The analysis of various adsorption sites and electronic properties reveals the catalytic potential of MoP(001) surface for CO2 activation.
JOURNAL OF CO2 UTILIZATION
(2022)
Article
Chemistry, Multidisciplinary
Junjun Wang, Xin Huang, Honglin Zhang, Linqing Wang, Weijiu Huang, Shaofu Kuang, Fuxiang Huang
Summary: The study investigated the peeling process of coatings by using first-principles calculations to analyze the work of adhesion, interface energy, and electronic structure. Results showed that the diamond-Si interface exhibited better performance, while the Ti-Ti interface was most prone to deformation, and the Si-Ti interface was more likely to delaminate.
JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
(2021)
Article
Materials Science, Multidisciplinary
Fuzhu Liu, Xiangdong Ding, Jun Sun
Summary: Uranium mononitride (UN), a promising nuclear fuel, suffers from surface oxidation and initial corrosion during storage and operation. This study investigates the interactions between adsorbates and different UN surfaces using density functional theory calculations. It is found that O2 molecules dissociate spontaneously on these surfaces, while H2O molecules weakly adsorb to U atoms. The competition between U-O and U-N interactions leads to the formation of uranium cavities on the surface. The insights gained from this study enhance our understanding of the initial oxidative corrosion of UN surfaces.
JOURNAL OF NUCLEAR MATERIALS
(2023)
Article
Chemistry, Physical
Gianfranco Ulian, Daniele Moro, Giovanni Valdre
Summary: This study focuses on the interaction between water and a single layer of (001) pyrophyllite surface. The adsorption of water molecules is found to be driven by van der Waals interactions, leading to self-assembly as water content increases. The results are in good agreement with previous data and have potential applications in mineralogy and petrography.
APPLIED CLAY SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Soon-Dong Park, Sung Youb Kim
Summary: In this study, we used spin-polarized density functional theory to analyze the properties of the Cr(001)/Al(001) structure, and found that the interface can be classified into three forms: bcc, bridge, and top. The total density of states of the structures is mainly influenced by the Cr (d) orbitals. The analysis of the mechanical properties showed that deformation mainly occurs in the Al region regardless of the interface type.
Article
Chemistry, Physical
Amit Sahu, Julien Parize, Celine Dupont
Summary: In this study, maghemite, the second most stable iron oxide, was investigated using a DFT+U approach. The relative stability of different surface terminations from the (001) and (111) planes were discussed, allowing the discrimination of preferred terminations among oxygen vs. iron, with octahedral or tetrahedral cations sites, etc. The strain effect induced by lattice mismatch was considered to move towards epitaxial growth of maghemite on a Pt substrate, resulting in a change in stability and indicating that the growth of the (111) surface will be favored over the one of the (001) on the Pt substrate due to numerous Pt-O interactions. Various electronic properties such as bond-lengths, bonding, charges, and density of states were analyzed to understand the nature and stability of the surfaces, showing that for surfaces, bandgaps are smaller than bulk, with a higher deviation for (001) than for (111) surfaces.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Physical
A. Benbella, I. Matrane, M. Badawi, S. Lebegue, M. Mazroui
Summary: This study investigates the adsorption behavior of pyridine and thiophene molecules on clean and doped Rh-Cu (100) and Pt-Cu (100) surfaces using density functional theory calculations. The results show that the adsorption energy of thiophene is significantly increased after alloying the Cu surface with an Rh tetramer, while the adsorption energy of pyridine is also enhanced after substituting the Cu atoms with an Rh tetramer. Bader charge analysis and electron density difference calculations confirm the charge transfer and accumulation between the surface atoms and the molecules during the adsorption process.
Article
Engineering, Electrical & Electronic
Edgar Daniel Sanchez Ovalle, Edgar Martinez-Guerra, Noboru Takeuchi, Rodrigo Ponce-Perez
Summary: Using first-principles calculations and thermodynamics criteria, we explored the structural and electronic properties of the AlP(001) surface with 18 different surface reconstructions. Our results identified five stable surface reconstructions, exhibiting semiconductor behavior except for the (2 x 2) P-dimer surface, which showed metallic behavior. The electron localization function profiles demonstrated the covalent nature of the Al-P and P-P bonds, while the Al-Al interaction was metallic. This study provides insights into possible surface reconstructions in AlP compounds and their potential applications in developing diluted magnetic semiconductors.
ACS APPLIED ELECTRONIC MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Huiru Yang, Xueting Liu, Anqi She, Zhao Zhao, Fangping Zhou, Li Niu, Haibo Li, Ming Feng, Dandan Wang
Summary: DFT calculations were used to study direct CH4 catalytic conversion over MoP (001) surface. It was found that introduction of N-2 would promote the conversion of CH4 into C-2 hydrocarbons, while inhibiting H-2 formation and leading to the formation of NH3. On the surface, N-2 dissociates into N* and influences the decomposition of CH4, ultimately resulting in the formation of C-2 hydrocarbons.
MATERIALS CHEMISTRY AND PHYSICS
(2022)
Article
Spectroscopy
Vinay Sharma, Sebastian Schluecker, Sunil K. Srivastava
Summary: Despite extensive scientific efforts to understand the exact nature of hydrogen bonding in Pyridine aqueous solutions, the exact mechanism causing the blue-shift in Py ring breathing mode has remained unclear so far. This study investigates the causes of the blue-shift by using density functional theory (DFT) to analyze electronic charge redistribution in Py-water complexes. Analysis suggests that the interaction between nitrogen lone pair in Py and hydrogen atom in water leads to a net charge transfer, resulting in depopulation of sigma* (C-C) orbitals and ultimately strengthening of local C-C force constants.
JOURNAL OF RAMAN SPECTROSCOPY
(2021)
Article
Energy & Fuels
Siyu Chen, Juanqin Li, Quan Zhu, Zerong Li
Summary: In this study, the thermodynamics and initial pyrolysis kinetics of five strained polycyclic hydrocarbons were investigated using quantum chemical computations. The results showed that ring bond breaking reactions were more energetically favorable than bridge bond breaking reactions. The studied reactions were divided into different classes based on the size of the rings and the types of carbon atoms, and reaction rate rules were established for each class. The studied strained polycyclic hydrocarbons had higher thermodynamic properties and easier initial pyrolysis kinetics compared to JP-10.
Article
Chemistry, Physical
Peng Zhang, Haobin Tan, Zhongkai Wang, Lai Lyu, Chun Hu
Summary: Establishing structure-activity relationship is crucial for designing catalysts with low energy consumption and high efficiency in advanced oxidation processes. This study investigates the atomic mechanism of hydrogen peroxide dissociation and formation on different zinc chalcogenides. The catalytic activity of hydrogen peroxide on zinc chalcogenides is determined by the surface micro-engineering construction including surface orientation and heteroatomic doping. These findings not only provide a better understanding of the mechanism of hydrogen peroxide on zinc chalcogenides, but also offer guidance for the development of new catalytic oxidation systems.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Physical
Honglin Li, Shoufu Cao, Hongman Sun, Yonglian Lu, Ying Zhang, Xiaoqing Lu, Jingbin Zeng, Zifeng Yan
Summary: In this study, Cu-based/CxNy catalysts were fabricated to improve the selectivity of C2H4 in CO2RR, overcoming the selectivity and stability issues of Cu catalyst. The precise tailoring of the synergistic effect between different Cu species and carbon nitride hybrids enabled the precise control of the product selectivity.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Xiaoqing Lu, Hui Xu, Tianfang Yang, Xiaodong Chen, Zhi Cheng, Qi Hou, Xiaojing Lin, Siyuan Liu, Shuxian Wei, Zhaojie Wang
Summary: Researchers have designed a controllable MoS2-coated nano-cube of Co3+-rich CoFe Prussian blue analogues as an oxygen evolution reaction (OER) electrocatalyst. This electrocatalyst, named CoIIIFe-PBA/MoS2, exhibits an extremely low overpotential of 306 mV at a current density of 100 mA cm-2, a small Tafel slope of 36.2 mV dec-1, and excellent stability for OER. Spectroscopic characterizations reveal that the Co3+ species in CoIIIFe-PBA/MoS2 originate from charge transfer at the CoFe-PBA and MoS2 core-shell interface, promoting electron accepting and enhancing electrochemical activity.
JOURNAL OF ALLOYS AND COMPOUNDS
(2023)
Article
Electrochemistry
Zhaojie Wang, Yizhu Shang, Hongyu Chen, Shoufu Cao, Qiuying Zhu, Siyuan Liu, Shuxian Wei, Xiaoqing Lu
Summary: The unique crystal structure and active electronic properties of a Cu-based catalyst are crucial for CO2RR. A series of copper hydroxyphosphate catalysts were synthesized and applied in CO2RR, where the concentration of OH- and NH4+ played an important role in the formation and aggregation of the crystal structures. Compared to Cu-2(OH)PO4, Cu-5(OH)(4)(PO4)(2) showed superior selectivity and activity for CO2RR to C2H4. With a Faradaic efficiency of C2H4 over 37.4% and outstanding stability, Cu-5(OH)(4)(PO4)(2) had more hydroxyl groups (-OH) and a higher catalytic area, providing increased interaction with CO2 molecules and more active sites for CO2RR. This work offers a new perspective for the design of stable Cu-based catalysts with tunable chemical environment for CO2RR.
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Hao Dong, Qiuying Zhu, Lu Wang, Xiaokun Yue, Hongxu Fang, Zhaojie Wang, Siyuan Liu, Shuxian Wei, Xiaoqing Lu
Summary: The distribution and connectivity of pores in shale reservoirs have a significant impact on CO2-enhanced oil recovery (CO2 EOR) in shale. Molecular dynamics simulation was used to investigate the microscopic mechanism of CO2 EOR in shale nanopores with different pore width distributions and connectivity. The results showed that pore connectivity has a significant effect on oil displacement, with the recovery efficiency being highest for connected pores, followed by double pores and single pores. The results provide theoretical support for the study of CO2 EOR in shale with different pore width distributions and connectivity, as well as the exploitation of shale oil.
Review
Chemistry, Physical
Hongyu Chen, Shoufu Cao, Lu Wang, Xiaojing Lin, Qiuying Zhu, Yizhu Shang, Shuxian Wei, Siyuan Liu, Zhaojie Wang, Baojun Wei, Xiaoqing Lu
Summary: The synthesis of boron-doped amorphous zinc oxide with or without antimony nanoparticles embedding was reported. The introduction of antimony nanoparticles led to a switching of product from CO to formate in carbon dioxide reduction, which was attributed to the weakened charge interaction on zinc atoms by antimony.
Article
Chemistry, Physical
Lianming Zhao, Yanfu Tong, Yanping Ding, Weichao Kong, Jianjun Wang, Bingyu Li, Yuchao Zhen, Jing Xu, Wei Xing
Summary: By density functional theory calculations, the alkaline hydrogen oxidation performance of heterostructures of nickel with transition metal nitrides (Ni/TMNs) was systematically studied. It was found that the optimized H* and OH* adsorption at heterojunction interfaces significantly accelerated the recombination of H* and OH*, resulting in high hydrogen oxidation activity. Among all catalysts, Ni/δ1-MoN showed the optimum activity.
SURFACES AND INTERFACES
(2023)
Article
Chemistry, Physical
Sen Liu, Maohuai Wang, Shuxian Wei, Siyuan Liu, Zhaojie Wang, Chi-Man Lawrence Wu, Daofeng Sun, Xiaoqing Lu
Summary: The study explored the use of metal-organic frameworks (MOFs) as CO2 capture adsorbents. It was found that by introducing functional groups, modifying pore size, and considering steric hindrance, the CO2 capture performance of MOFs can be significantly enhanced. The highest CO2 capture capacity was achieved by UPC-OSO3-steric, with selectivities of 1142.41 (CO2 over N2) and 507.42 (CO2 over CH4) at 1.0 bar, 298 K. The mechanisms of the synergistic effects were elucidated through theoretical calculations analyzing pore characteristics, gas distribution, and intermolecular interactions.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Chemistry, Physical
Shoufu Cao, Yuchun Liu, Yuying Hu, Jiao Li, Chunyu Yang, Zengxuan Chen, Zhaojie Wang, Shuxian Wei, Siyuan Liu, Xiaoqing Lu
Summary: In this study, Ti2CO2 and O vacancy containing Ti2CO2 MXene-based single atom catalysts (SACs) were explored for electrocatalytic CO2 reduction reaction (CO2RR) to CO. Ni-Ov-Ti2CO2 showed promising results as a catalyst for CO2RR to CO, with a high limiting potential and selectivity. Furthermore, a novel activity descriptor based on the TM-Ti-O group valence state was proposed for CO2RR. This work highlights the potential of Ti2CO2-based Ni SAC as a catalyst for CO2RR and provides a design principle for MXene-based SACs.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Materials Science, Multidisciplinary
Shoufu Cao, Hongyu Chen, Jiao Li, Zengxuan Chen, Chunyu Yang, Shuxian Wei, Siyuan Liu, Zhaojie Wang, Xiaoqing Lu
Summary: In this study, first-principle calculations were used to investigate the mechanism of CO2 reduction reaction on single metal atoms anchored to nitrogen-containing carbon. The results show that nitrogen-containing carbon effectively immobilizes and activates metal centers, with higher activity observed on M-NC surfaces compared to MPc surfaces. The study provides profound insights into the coordination environment and the role of various metal centers in M-N-x materials.
JOURNAL OF MATERIALS SCIENCE
(2023)
Article
Chemistry, Physical
Xiaoqing Lu, Yuying Hu, Shoufu Cao, Jiao Li, Chunyu Yang, Zengxuan Chen, Shuxian Wei, Siyuan Liu, Zhaojie Wang
Summary: In this study, a novel two-dimensional transition metal boride, MoB, was found to exhibit excellent catalytic activity and selectivity for the CO2 reduction reaction. It shows great potential as a catalyst for mitigating greenhouse effect and energy shortage.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Xiaofei Wei, Huakai Xu, Chuanhai Jiang, Zhifei Wang, Yuguo Ouyang, Chunyu Lu, Yuan Jing, Shiwei Yao, Xiaoqing Lu, Fangna Dai
Summary: Metal atom dispersed catalysts with high catalytic activity and accurate active sites are promising for electrocatalytic CO2 reduction reactions. Fe atom catalysts with pairs of Fe atoms at different distances were constructed and the effect of distance on catalytic performance was investigated. The FeN4-D1 structure exhibited good selectivity and catalytic activity for producing CO due to its structural stability and activation effect for CO2. Moreover, the FeN4-D1 structure had superior catalytic performance and selectivity for the CO2RR to ethanol by promoting the C-C coupling process through the modification of the interaction between the FeN4-D1 structure and *CO intermediates.
MATERIALS CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Physical
Zengxuan Chen, Shoufu Cao, Jiao Li, Chunyu Yang, Shuxian Wei, Siyuan Liu, Zhaojie Wang, Xiaoqing Lu
Summary: This study reveals that introducing different numbers of sulfur atoms into N coordination can enhance the structural stability and catalytic activity of the catalyst, accelerating the CO2 reduction reaction. The sulfur atom substitution has significant influence on the product selectivity and catalytic performance.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Review
Chemistry, Multidisciplinary
Xingheng Zhang, Qi Hou, Shoufu Cao, Xiaojing Lin, Xiaodong Chen, Zhaojie Wang, Shuxian Wei, Siyuan Liu, Fangna Dai, Xiaoqing Lu
Summary: This review presents recent advances of cobalt phosphate (CoPi) based catalyst in the oxygen evolution reaction (OER) process of water splitting, including structural composition, synthesis methods, and OER enhancement. CoPi has attracted great attention due to its low cost, good stability, high catalytic activity, and redox properties.
Article
Chemistry, Physical
Zhaojie Wang, Qi Hou, Xingheng Zhang, Huanhuan Liu, Xiaojing Lin, Hongyu Chen, Ruidong Ding, Shuxian Wei, Xiaoqing Lu, Siyuan Liu
Summary: This study proposes a method of enhancing the activity of catalysts for alkaline water electrolysis through etching and doping. The etching of silver-doped cobalt phosphate catalysts with alkaline solutions can increase the number of active sites and electrical conductivity, thereby significantly improving electrocatalytic performance. The catalyst exhibits excellent stability and efficient electrolysis performance under industrial conditions.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Physical
Lili Fan, Xiaofei Wei, Xuting Li, Zhanning Liu, Mengfei Li, Shuo Liu, Zixi Kang, Fangna Dai, Xiaoqing Lu, Daofeng Sun
Summary: This study reports a phosphorus-doped Fe-N-C catalyst with penta-coordinated single atom sites for efficient oxygen reduction. The catalyst exhibits remarkable ORR activity and stability in alkaline, neutral, and acidic media.
