Article
Engineering, Environmental
Peng Liu, Yilian Kong, Xiaoliang Liang, Yuxi Liao, Tan Li, Daoyong Tan, Runliang Zhu, Mingli Fu, Steven L. Suib, Daiqi Ye
Summary: Biogenic isoprene is a significant pollutant for regional air quality. The substitution of Fe for Mn in cryptomelane plays a crucial role in enhancing the oxidation of isoprene. The adsorption of isoprene on cryptomelane is influenced by environmental temperature.
JOURNAL OF HAZARDOUS MATERIALS
(2022)
Article
Chemistry, Physical
Nan Li, Jin Wang, Junxia Wang, Yan Wang, Yuhao Fu, Jianzhou Zhao
Summary: In this work, the adsorption mechanism of uranyl on montmorillonite was studied using first-principles DFT + U calculation. The adsorption energy, geometry configuration, and electronic properties of the systems were systematically investigated. It was found that the adsorption of uranyl depended on the number of water ligands and their positions in the interlayer of montmorillonite. The study also showed that the migration of uranyl within the interlayer could be inhibited by hydrogen bonding with water ligands.
APPLIED SURFACE SCIENCE
(2023)
Article
Construction & Building Technology
Yue Zhang, Qingqing Xu, Ming Sun, Chuansheng Xiong, Pan Wang, Zheng Chen, Guoxing Sun, Jing Guan, Zhiheng Ding, Mengmeng Li, Dongshuai Hou
Summary: The study found that vitamin B3 formed the most stable adsorption structure on the gamma-FeOOH surface with the lowest adsorption energy. Van der Waals force and solvent effect play important roles in the adsorption process, and stronger adsorption is indicated by more chemical bond formations.
CONSTRUCTION AND BUILDING MATERIALS
(2021)
Article
Chemistry, Applied
Lu Chen, Xinping Wu, Xueqing Gong
Summary: In this study, density functional theory calculations were used to investigate the reactivity of Pd- and Zr-doped CeO2(111) surfaces at different locations. The results show that both Pd and Zr doping can activate the surface lattice O and lower the energy barriers of CO oxidation. However, the promotion effect of Zr doping is limited to the first surface layer, while Pd doping can greatly enhance surface activity even below the surface. CO2 can be directly generated on Pd-doped surfaces through the reaction between CO and surface O, while on Zr-doped surfaces, the formation of surface intermediate CO2d- may restrict the release of CO2 by further oxidation to carbonates. Electronic analysis reveals that the doped Pd exists as Pd4+ and has stronger electron affinity, facilitating the transformation from Pd4+ to Pd2+ and the direct formation of CO2 during CO oxidation. Published by Elsevier B.V. All rights reserved.
JOURNAL OF RARE EARTHS
(2023)
Article
Chemistry, Inorganic & Nuclear
Tao Chen, Huanhuan Dong, Tong Liu, Li Zhou, Dengjiang Fu, Beibei Pang, Jie Lian, Tao Ding, Wei Zhang, Rong He, Wenkun Zhu
Summary: In this study, a directional half-wave rectified alternating current electrochemical method was used to confine oxygen-rich uranium precursors over ultrathin 2D GO nanosheets, preparing uranium catalysts. The as-prepared uranium catalysts exhibited a considerable Faradaic efficiency of 12.7% for NH3 and an NH3 yield rate of 18.7 μgh(-1) mg(-1) for N-2 electroreduction. Operando XAS and isotope-labeling FTIR further revealed the preferred nitrogen adsorption reaction intermediate N-(2O(ax)-1 U-4O(eq)) and confirmed the key *N2Hy intermediate species derived from the fed N-2 gas. Theoretical simulations demonstrated that the U-O atomic interface originated from U 5f-O 2p orbital hybridization can accumulate partial charge from GO, facilitating N Ndissociation and reducing the thermodynamic energy barrier of the first hydrogenation step.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Ho Viet Thang
Summary: Doping heteroatoms is an effective method for enhancing the electronic properties of ZnO materials for desired applications. This study investigates the effects of different dopant metals on the electronic and adsorption properties of ZnO(1010) using DFT + U calculations. The research shows that Cu dopant significantly enhances the adsorption characteristics of ZnO materials. This study will be beneficial for designing appropriate materials for adsorption and catalytic applications.
Article
Chemistry, Multidisciplinary
Peace P. Mkhonto, Phuti E. Ngoepe
Summary: In this study, the crystal structure and surface stability of Cooperite (PtS) were investigated using computational modeling methods. The results revealed the reconstruction mechanisms and stability differences of different surfaces, providing an explanation for its specific crystal morphology.
Article
Chemistry, Multidisciplinary
David C. Grinter, Michael Allan, Hyun Jin Yang, Agustin Salcedo, Gustavo E. Murgida, Bobbie-Jean Shaw, Chi L. Pang, Hicham Idriss, M. Veronica Ganduglia-Pirovano, Geoff Thornton
Summary: A Ce=O terminated ceria surface was observed in this study, revealing a key feature in the reconstruction of ceria islands and potentially shedding light on the unique catalytic properties of ceria-based systems.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Materials Science, Multidisciplinary
Dario Mastrippolito, Jing Wang, Gianni Profeta, Luca Ottaviano
Summary: In this study, the magnetic properties of two-dimensional CrCl3 systems were investigated using density functional theory and Monte Carlo simulations. It was found that the introduction of Cl vacancies leads to a linear increase in magnetic moment, strengthening the ferromagnetic state and increasing the Curie temperature. Additionally, the presence of oxygen impurities results in the formation of a stable ordered phase, with antiferromagnetic coupling between chromium and oxygen atoms, giving rise to a two-dimensional ferrimagnetic hexagonal lattice system with a high magnetic ordering temperature.
JOURNAL OF PHYSICS-MATERIALS
(2022)
Article
Chemistry, Physical
Oscar Hurtado-Aular, Rafael Anez, Anibal Sierraalta
Summary: This study investigates the adsorption behavior of Cu, Ag, or Au on the surface of WO3, as well as the adsorption of CO molecules. The results show that the adsorption of Cu, Ag, and Au atoms induces changes in the surface electronic structure, while the adsorption of CO leads to a reduction in band gap. The findings provide insights for the potential applications of WO3 in gas sensing chemistry and photocatalysis.
Review
Chemistry, Applied
Tariq Bashir, Sara Adeeba Ismail, Jiaqi Wang, Wenhao Zhu, Jianging Zhao, Lijun Gao
Summary: This paper summarizes the nature of chemical bonding in MXenes and discusses the surface terminators of several MXenes. The study finds that =O, -OH, -F, and -Cl are typical MXene surface terminators, but recent investigations show that -OH cannot be considered an intrinsic termination species in MXenes. Additionally, the paper discusses different etching approaches for MXene synthesis, the dependence of MXene conductivity on terminating groups, and the emission of gaseous products during chemical transformations.
JOURNAL OF ENERGY CHEMISTRY
(2023)
Article
Energy & Fuels
Jun Liu, Tao Wang, Nan Shi, Jing Yang, Mohamed A. Serageldin, Wei-Ping Pan
Summary: This work presents a method for increasing VOC removal from flue gas. By using a mechanochemical synthesis method and adding a solid organic acid ligand (OAL), the catalyst, Ce-Mn-OFA, showed improved oxidation and adsorption activity, making it a potential solution for VOC removal.
Article
Chemistry, Applied
E. P. Munzhelele, W. M. Gitari, W. B. Ayinde, R. Mudzielwana
Summary: This study presents the synthesis of cerium doped poly(-para-phenylenediamine) composite (Ce-pPD) and evaluates its potential towards the removal of fluoride, arsenic, and pathogens from aqueous solution. The results show that Ce-pPD has a strong affinity towards fluoride and a high adsorption capacity, and also exhibits antimicrobial activity against various pathogens.
REACTIVE & FUNCTIONAL POLYMERS
(2022)
Article
Chemistry, Physical
Vadim D. Knyazev
Summary: In this study, the kinetics of ten reactions involving substituted methyl radicals producing a carbonyl compound and hydroxy radical were computationally investigated using quantum chemistry, transition state theory, and master equation / RRKM. The effects of Cl, F, and CF3 substitution were quantified. It was found that Cl substitution led to a decrease in rate constants. The first F substitution lowered the energy barrier and subsequently increased the rate constants, while the second F substitution left the energy barrier unchanged and partially reversed the trend in rate constants. CF3 substitution, on the other hand, increased the energy barrier and decreased the rate constants. Additionally, the rate constants of ten R + O2 -> RO + O reactions were estimated based on detailed balance.
CHEMICAL PHYSICS LETTERS
(2022)
Article
Chemistry, Physical
Le Zhang, Bo Sun, Qili Zhang, Haifeng Liu, Kezhao Liu, Haifeng Song
Summary: This study investigates the differences in adsorption behaviors of H2O and CO2 on PuO2 surface, mainly attributed to the hydrogen bonds and Coulomb interactions between the adsorbed molecules.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Physical
Hao Zhou, Lu Chen, Yong Guo, Xiaohui Liu, Xin-Ping Wu, Xue-Qing Gong, Yanqin Wang
Summary: The Ru/NbOx catalysts show a great potential in cleaving C-sp2-C-sp3 bonds in lignin and aromatic plastics due to their ability in hydrogen activation and strong binding to benzene rings. Furthermore, NbOPO4 catalyst with oxygen vacancies and Bronsted acidity demonstrates unique capability in cleaving C-sp2-C-sp3 bonds and hydrogenolysis of robust compounds, indicating a promising direction for designing cost-effective metal-free hydrogenolysis catalysts.
Article
Nanoscience & Nanotechnology
Cheng-Long Ma, Xue-Rui Yang, Zhi-Qiang Wang, Wei Sun, Lin Zhu, Li-Mei Cao, Xue-Qing Gong, Ji Yang
Summary: This study evaluates the structural and electronic-state characteristics of long-range disordered amorphous iridium-based oxides and their performance in oxygen evolution reaction (OER). It demonstrates that the ultrahigh OER performance in acidic media is driven by the more d-hole-containing electronic state of Ir-V created by cationic vacancies. Moreover, the high edge-shared [IrOx]-[IrOx] motif proportion structure achieves a stable OER process similar to IrO2.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Physical
De-Ren Chu, Zhi-Qiang Wanga, Xue-Qing Gonga
Summary: This study investigated the direct CO oxidation behavior on four types of CeO2(111) surface steps using density functional theory (DFT) calculations. The results showed that CO adsorption can be enhanced at step edges through the alignment of C-O and surface Ce-O bonds. The reactivities of step edges on the CeO2(111) surface were found to be similar to those of the corresponding extended facets. Oxygen sites at step edges with lower coordination numbers were found to have smaller vacancy formation energies and higher reactivities. Additionally, the Ce 4f orbital energy level was found to decrease after CO adsorption on a specific type of step, contributing to its superior catalytic activity towards CO oxidation. The unique role of CeO2(111) steps in influencing reactant adsorption, activation barriers, product desorption, and overall CO catalytic oxidation activities was revealed. These findings may inspire further research on the structure-reactivity relationships over surface defect sites on rare-earth oxide catalysts.
Article
Chemistry, Physical
Zheng-Li Xie, Dong Wang, Xue-Qing Gong
Summary: This study reveals the complete reaction mechanism and rate-determining steps of nitrate reduction on Pt/TiO2 catalyst. By regulating the charge density of Pt, the dissociation and hydrogenation steps of the reaction can be modified, leading to improved activity. Doping Zn or Cu into TiO2 is proposed as an effective strategy to enhance the nitrate reduction activity.
Article
Chemistry, Physical
Fei Li, Jian-Fu Chen, Xue-Qing Gong, P. Hu, Dong Wang
Summary: This study investigates the significance of surface structures in altering the photooxidation functions of titanium dioxide (TiO2) in aqueous environments. By developing a solution simulation method, the researchers identify a complete mechanism for the photocatalytic oxygen evolution reaction (OER) and determine the leading reaction pathway based on the concentration of photoholes reaching the surface. The results also reveal the importance of proper surface structures in achieving efficient catalysis.
Article
Multidisciplinary Sciences
Hui Zhou, Xin-Ping Wu, Xue-Qing Gong
Summary: In this study, density functional theory calculations were used to analyze the reconstruction and adsorption phenomena on polar CeO2 surfaces. The formation of pocket-like structures was found to increase surface stability and promote the adsorption and dispersion of metal atoms. This study provides new models for understanding surface reconstruction and adsorption.
ADVANCED THEORY AND SIMULATIONS
(2022)
Article
Chemistry, Multidisciplinary
Jinhong Jia, Jingjiang Liu, Zhi-Qiang Wang, Tao Liu, Peiyao Yan, Xue-Qing Gong, Chengxi Zhao, Linjiang Chen, Congcong Miao, Wei Zhao, Shanshan (Diana) Cai, Xi-Cun Wang, Andrew Cooper, Xiaofeng Wu, Tom Hasell, Zheng-Jun Quan
Summary: Inverse vulcanization (IV) is a technique that converts elemental sulfur into sulfur-rich functional polymers. Previous methods required harsh reaction conditions, limiting the range of feasible crosslinkers. This study introduces a new photoinduced IV method that allows reaction at ambient temperatures, significantly expanding the range of substrates and products, and providing sustainable alternatives for environmentally harmful plastics.
Article
Chemistry, Physical
Tao Tong, Mark Douthwaite, Lu Chen, Rebecca Engel, Matthew B. Conway, Wanjun Guo, Xin-Ping Wu, Xue-Qing Gong, Yanqin Wang, David J. Morgan, Thomas Davies, Christopher J. Kiely, Liwei Chen, Xi Liu, Graham J. Hutchings
Summary: The physicochemical properties of Pt/CeO2 catalysts were varied to investigate their impact on the hydrogen-borrowing amination of alcohols. It was found that the Pt precursor and CeO2 support properties strongly influenced catalytic performance. The most active catalyst exhibited linearly structured Pt species, which were more effective for the rate-determining step of cyclopentanol dehydrogenation compared to Pt clusters and nanoparticles. This study not only provides insights into desirable catalytic properties for hydrogen-borrowing amination but also has broader relevance to related fields.
Article
Chemistry, Physical
Hui Zhou, Dong Wang, Xue-Qing Gong
Summary: By performing density functional theory calculations, it was found that the composite catalysts of inverse CeOx/Cu(111) can produce more active hydride species compared to CeO2 or Cu alone. This is mainly due to the efficient combination of the unique structural feature of CeOx islands and the electronic promotion from Cu. Additionally, modifying the Cu(111) surface with pyridine molecules can enhance the thermo- and dynamical stabilities of the hydride species.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Yan-Ping Zhang, Zi-Xiang Su, He-He Wei, Zhi-Qiang Wang, Xue-Qing Gong
Summary: In this study, the researchers systematically investigated the oxygen reduction reaction (ORR) on various Pt-Bi surfaces using density functional theory calculations. They found that the introduction of Bi changes the determining step of ORR and identified the hydroxy adsorption free energy (GOH*) as a descriptor for ORR activity. The researchers also discovered that the combination of tensile strain introduced by Bi and electron transfer between Pt and Bi affects the d-band position of Pt, leading to the highest ORR activity on PtBi(100), even exceeding that of Pt(111).
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Multidisciplinary Sciences
Bin Shao, Zhi-Qiang Wang, Xue-Qing Gong, Honglai Liu, Feng Qian, P. Hu, Jun Hu
Summary: The integrated CO2 capture and conversion (iCCC) technology is a promising cost-effective approach for Carbon Neutrality. The lack of molecular consensus about the synergistic effect between adsorption and in-situ catalytic reaction hampers its development. In this study, the synergies between CO2 capture and in-situ conversion are illustrated through high-temperature Calcium-looping and dry reforming of methane processes.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Cong Fu, Fei Li, Zongfang Wu, Feng Xiong, Junfa Zhu, Xue-Qing Gong, Weixin Huang
Summary: A trace amount of potassium dopant is found to restructure the surface of anatase TiO2(001) single crystal, changing the termination from molecule termination to oxygen termination. The molecule-terminated surface shows (photo)catalytic activity, while the oxygen-terminated surface is inert.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Renjie Zhou, Lipeng Yang, Zhengda Chen, Li Jiang, Tuan Liu, Zhiqiang Wang, Xinyi Huang, Qiuning Lin, Xueqing Gong, Yi Yang, Linyong Zhu
Summary: Photoactivated fluorophores (PAFs) have great potential as imaging tools for subcellular structures and dynamic biological processes. However, the current photoremovable protecting groups (PPGs) used in PAF construction have limitations in terms of excitation wavelength and efficiency. In this study, a new class of coumarin-based PPGs with electron-rich thiophene derived substitutions was developed to address these limitations. The modified PPGs showed redshifted absorption and increased photolysis efficiency, enabling efficient photolysis even under weak blue light. The resulting PAF exhibited fast photoactivation, low background signal, and high signal-to-noise ratio in fluorescence imaging. It is anticipated that these superior photolysis properties make the PPGs a novel platform for constructing photoresponsive systems in various applications.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Yan-Ping Zhang, Zi-Xiang Su, He-He Wei, Zhi-Qiang Wang, Xue-Qing Gong
Summary: Reducing the use of Pt in proton exchange membrane fuel cells is a significant interest for both academia and industry. This study investigated the oxygen reduction reaction (ORR) on various Pt-Bi surfaces using density functional theory calculations. The introduction of Bi altered the determining step of ORR and the hydroxy adsorption free energy (GOH*) was found to be an indicator of ORR activity, with 0.74 eV being the optimal GOH* value. It was also discovered that the strain induced by Bi and electron transfer between Pt and Bi influenced the d-band of Pt, resulting in PtBi(100) having superior ORR activity compared to Pt(111).
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Xiang-Peng Tao, Xue-Qing Gong, Dong Wang
Summary: The study reveals the reaction mechanism of photocatalytic formaldehyde degradation and proposes an optimal degradation mechanism that harnesses the advantages of photogenerated holes and (OH)-O-center dot radicals. Additionally, the research also discovers the correlation between the catalytic and thermocatalytic reaction barriers of C-H bond activation and the polarity of C-H bonds.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
