Article
Chemistry, Physical
Shijiu Liu, Zhikang Zhou, Jianmin Chen, Yu Fu, Canying Cai
Summary: The adsorption and dissociation of CO2 on perfect and oxygen-deficient gamma-Al2O3(1 0 0) were studied using first-principles calculations. It was found that CO2 molecules physically absorb at perfect gamma-Al2O3(1 0 0) without decomposition. However, in the presence of oxygen vacancies, CO2 can directly decompose or adsorb at adjacent Al sites and then rotate to the oxygen vacancy for decomposition. The charge transfer between CO2 and the surface was analyzed to understand the effect of oxygen deficiency on CO2 adsorption and decomposition. Overall, the presence of oxygen vacancies promotes CO2 activation and has practical importance in catalytic CO2 conversion and controlling oxidation processes.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Physical
Shulan Zhou, Qiang Wan, Sen Lin
Summary: Density functional theory calculations were used to study H-2 dissociation and acetylene hydrogenation on Cu doped CeO2(111). The results showed that Cu doping promotes the formation of oxygen vacancy and creates Cu/O and Ce/O frustrated Lewis pairs. H-2 dissociation proceeds via a heterolytic mechanism with the help of Cu/O frustrated Lewis pair, while C2H2 hydrogenation can be catalyzed by Cu-H and O-H species. Cu doped CeO2(111) exhibits high activity and selectivity for acetylene hydrogenation.
Article
Materials Science, Ceramics
Qi Zhou, Shizhen Zhu, Zhuang Ma, Yanbo Liu, Ling Liu, Lihong Gao
Summary: Ceria is a potential candidate for high-temperature infrared stealth materials due to its high melting point, oxidation resistance, and low infrared emissivity. This study investigates the effect of oxygen vacancy concentration on the infrared emissivity of ceria. It was found that the emissivity decreases with increasing oxygen vacancy concentrations, which can be attributed to the increase in free carrier concentration, as confirmed by first-principles calculations.
CERAMICS INTERNATIONAL
(2022)
Article
Materials Science, Multidisciplinary
Yongsheng Zhao, Fengyun Yan, Yi An
Summary: The formation and properties of interfaces in composite materials are crucial for their preparation. This study investigated the adsorption behavior of copper atoms on the (111) surface of H-terminated diamond using first-principles calculations. The results showed that copper adsorption was not sensitive to the diamond surface and the interface formed was a metastable structure.
Article
Chemistry, Physical
Sung Gu Kang, Won Mook Choi
Summary: The performance of Sr-doped CeO2-delta(1 1 1) in adsorbing and reducing NO2 was systematically studied. The adsorption strength of NO2 on Sr-doped ceria can be tuned by strain and a promoter. The presence of the Al promoter enhances the adsorption of NO2 on Sr-doped ceria.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Analytical
Tong Li, Qi Wang, Zhou Wang
Summary: This study investigates the synergistic effect of crystal facets and heavily doped oxygen vacancies in CeO2 nanocrystals. It is found that the most stable CeO2 octahedron with heavily doped (111) facets demonstrates optimal non-enzymatic H2O2 sensing performance, indicating the significant influence of oxygen vacancies on different facets. The inclined distribution states of oxygen vacancies and the electronic transmission property clarify the synergistic effect of facet and oxygen vacancy.
Article
Materials Science, Multidisciplinary
Yang He, Biyao Sun, Lai Jiang, Xinlan Li, Yuning Ma, Kexin Wang, Peng Han, Shaowei Jin
Summary: First-principles calculations were used to investigate the impact of Ag doping on SnO2 sensing of H2S. The results showed that Ag doping enhanced the sensing performance of SnO2 semiconductors, leading to an increased sensitivity to H2S and improved sensor response capabilities.
Article
Materials Science, Multidisciplinary
Qi Zhang, Yongqi Chen, Jin Wang, Zhiping Lin, Xin Zhang, Huafeng Dong, Fugen Wu
Summary: The serial interaction of LiPSs intermediates on the surface of vacancy-defective MnO2 was investigated by first-principles calculation. Vacancy defects in MnO2 cause adjustments in electron density and increase polarization, creating favorable oxygen-vacancy traps for LiPSs. The presence of unpaired electrons enhances the interaction between vacancy-defective MnO2 and Li2Sn molecules, reducing the adsorption energy. Vacancy defects serve as effective nucleation sites, enhancing Li2S affinity, catalyzing LiPSs conversion, and improving shuttle effect and material utilization.
COMPUTATIONAL MATERIALS SCIENCE
(2023)
Article
Physics, Condensed Matter
Luca Brugnoli, Shingo Urata, Alfonso Pedone
Summary: Periodic density functional theory calculations were performed to investigate the absorption and decomposition of H2O2 on different models of ceria (111) surface. The results showed that on the clean surface, H2O2 decomposes through adsorption, deprotonation, and formation of peroxide anion. On the defective surface, H2O2 dissociation is driven by the healing of O vacancies. On the hydroxylated surface, H2O2 first adsorbs and then undergoes heterolytic dissociation.
JOURNAL OF PHYSICS-CONDENSED MATTER
(2022)
Article
Engineering, Chemical
Zhengyun Zhang, Lichuan Deng, Xiaolong Zhou
Summary: Density functional theory was used to investigate the adsorption behavior of fluoride molecules on pure, Co-doped and Pd-doped Ag(1 1 1) surfaces. Different adsorption behaviors were observed due to lattice change and charge transfer caused by doping. The adsorption energy, bond length, bond angle, Mulliken charge population, and charge density difference were analyzed. The research provides theoretical guidance for the design of efficient gas pollutant adsorption surfaces.
CHEMICAL ENGINEERING SCIENCE
(2023)
Article
Chemistry, Physical
Long Xie, Bin Hu, Riyang Shu, Zhipeng Tian, Ying Chen, Chao Wang
Summary: This study investigated the effect of different CeO2 morphologies on the catalytic performance of Ru/CeO2 catalysts in methanol reforming for hydrogen production. The results showed that the Ru/CeO2 catalyst with rod-shaped CeO2 exhibited better catalytic performance due to its larger surface area, which favored the dispersion of Ru metal sites and improved the interaction between Ru and CeO2 support.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Physical
Noah Baumann, Jinggang Lan, Marcella Iannuzzi
Summary: The first principles simulations of carbon dioxide adsorbed on the ceria (CeO2) (111) surface were discussed in terms of structural features, stability, charge transfer, and vibrational modes, using different density functional theory methods. The electronic structure of the reduced ceria surface was obtained by introducing oxygen vacancies, and bent CO2 configurations near the surface oxygen vacancy were identified as the most stable minima. The concentration of oxygen vacancies on the surface directly impacts the relative stability of potential adsorption configurations, and the vibrational analyses showed promising agreement with previous theoretical and experimental results.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Haohao Wang, Caiwei Yue, Jirui Du, Min Pu, Ming Lei
Summary: A density functional theory study was conducted to investigate the mechanism of nitrobenzene hydrogenation by a Ni-1/CeO2-x single-atom catalyst. The most favorable pathway for the hydrogenation of nitrobenzene to aniline by Ni-1/CeO2-x (111) was determined. The rate-determining step of the overall reaction was identified as the fourth hydrogen transfer step with an energy barrier of 1.24 eV.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Jacqueline Hidalgo-Jimenez, Taner Akbay, Tatsumi Ishihara, Kaveh Edalati
Summary: In this study, the high-pressure torsion method was used to stabilize the oxygen-deficient high-pressure phase of TiO2, columbite, as an active photocatalyst. The activity of columbite was found to be higher than that of the anatase phase. DFT calculations revealed that columbite has improved optical bandgap and light absorbance due to oxygen vacancies, as well as higher water adsorption energy and lower surface activation energy for water splitting.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Kai Yan, Chang Wen, Rui Li, Bohan Zhang, Tianyu Liu, Qian Liu, Zijian Zhou
Summary: In this study, CeO2 and Cu-doped CeO2 with different morphologies and crystallite sizes were synthesized to investigate their influence on the physical properties and photoresponse performance of CeO2 as well as the hydrogen production in PTC. Cu-doped CeO2 nanospheres with smaller crystallite size exhibited the best catalytic activity, generating the highest yield of H2. The change in physical properties was positively correlated with the yield, highlighting its importance in VOs consumption. The smaller crystallite size of the nanospheres facilitated thermochemical reaction by providing better porous properties and specific surface area, while the doping enhanced light absorption capacity and H2 yield of CeO2.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Physical
Zhansheng Lu, Yingjie Cheng, Dongwei Ma, Huijun Liang, Xiaobing Wang, Lin Yang, Zongxian Yang
Summary: The properties and behaviors of Fe@HAP and Fe/HAP were investigated using first-principles study, revealing that Fe@HAP can be stably anchored and enhance the ORR catalytic activity. The ORR process on Fe@HAP prefers the 4e pathway and the hydrogenated OH species tend to further hydrogenate.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Physical
Z. Wang, S. W. Fan, H. G. Piao, Z. S. Lu
Summary: 2D Mo2B is a stable metal phase with potential as an electrode material for ion batteries, and shows promise as a catalyst for hydrogen evolution.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Physical
Shamraiz Hussain Talib, Xiaohu Yu, Zhansheng Lu, Khalil Ahmad, Tongtong Yang, Hai Xiao, Jun Li
Summary: The study proposes a new strategy for NH3 synthesis using a transition metal single-atom catalyst anchored on a phosphomolybdic acid cluster under mild conditions, with the enzymatic pathway showing the highest efficiency. The Mo-1/PMA catalyst enhances N-2 adsorption, stabilizes N2H* species, and hinders the hydrogen evolution reaction, leading to improved eNRR selectivity. The results provide valuable insights for NH3 synthesis with high efficiency and low cost using single-atom catalysts at ambient temperature.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Physics, Applied
Yudong Pang, Zhansheng Lu, Shamraiz Hussain Talib, Xinyuan Li, Mingyang Wang, Xilin Zhang, Zongxian Yang, Ruqian Wu
Summary: This study investigates the effects of heteroatom doping and charge variation on the ability of MoS2 substrate to capture Na ions in sodium-ion batteries using first-principles calculations. The results show that Al- or Si-doped MoS2 can serve as good electrode materials with high theoretical capacity.
PHYSICAL REVIEW APPLIED
(2022)
Article
Physics, Multidisciplinary
Xinyuan Li, Yudong Pang, Mingyang Wang, Xilin Zhang, Zhansheng Lu, Zongxian Yang
Summary: Currently, MXenes have been recognized as a promising choice for Na-ion battery electrode materials due to their excellent energy storage and electrical conductivity. Among these, dual transition metal MXenes have gained attention as anode materials for Na-ion batteries because of their superior properties. In this study, we compared the performance of TiNbC-based dual transition metal MXenes and Nb2C-based single transition metal MXenes as anode materials for Na-ion batteries through density functional theory calculations. The results showed that TiNbC, TiNbCO2, Nb2C, and Nb2CO2 exhibited great potential as anode materials due to their low diffusion barrier and high Na capacity. Furthermore, TiNbC-based MXenes demonstrated better adsorption performance, diffusion rate, and theoretical storage of Na atoms compared to Nb2C-based MXenes, which was attributed to the synergistic effect between Ti and Nb. This discovery provides valuable insight for the development of high-performance MXenes-based anode materials for Na-ion batteries.
Article
Nanoscience & Nanotechnology
Yubo Liang, Cailing Wu, Songjie Meng, Zhansheng Lu, Runyao Zhao, Huiyong Wang, Zhimin Liu, Jianji Wang
Summary: In this study, Ag single-atom catalysts (SACs) supported on CeO2 (Ag-1/CeO2) were prepared using a new in situ adsorption-reduction method. The Ag single atoms were anchored on CeO2 through strong metal-support interaction (SMSI) and were accompanied by three interfacial oxygen vacancies. Ag-1/CeO2 exhibited high performance in the electrocatalytic CO2 reduction reaction (CO2RR), with a high CO faradaic efficiency (FE) of >95% and a turnover frequency (TOF) value of 50,310 h(-1) at FECO = 99.5% in H-cells. Notably, Ag-1/CeO2 achieved an industrial-grade current density of 403 mA cm(-2) with a high FECO of 97.2% in flow cells. Experimental results and density functional theory calculations revealed that the superior performance was mainly attributed to the existence of interfacial oxygen vacancies, which formed Ag-O-Ce3+ atomic interfaces and activated the Ce3+-O structures as the synergistic active center of Ag, thereby promoting CO2 adsorption and activation and reducing the reaction potential barrier of *COOH-to-*CO.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Physics, Applied
Peng Lv, Wenjing Lv, Donghai Wu, Gang Tang, Xunwang Yan, Zhansheng Lu, Dongwei Ma
Summary: This study investigates ultrahigh-density double-atom catalysts (DACs) and confirms their existence experimentally, showing low overpotentials and high oxygen-reduction reaction (ORR) activity.
PHYSICAL REVIEW APPLIED
(2023)
Article
Chemistry, Physical
Ayaz Mahsud, Muhammad Arif, Wasim Ullah Khan, Tianhao Zhang, Sajjad Hussain, Mohammad Azam, Zhansheng Lu
Summary: This study compared single-atom iron-doped nitrogen-based graphene with bimetallic iron-doped nitrogen-based graphene and found that the bimetallic atoms can change the surrounding nitrogen atoms and bond length of iron. The research suggests that in catalytic activity, not only d-orbitals along the z-direction play a vital role, but also the d-band center and magnetic moment have a projecting role in boosting catalytic activity.
MOLECULAR CATALYSIS
(2023)
Article
Chemistry, Physical
Mingyang Wang, Jianjun Mao, Yudong Pang, Xilin Zhang, Haiyan Wang, Zongxian Yang, Zhansheng Lu, Shuting Yang
Summary: This work reports on an effective strategy for enhancing the electrochemical performance of Li-S batteries by doping single atom Zn on the S-terminated Ti2C MXenes. The study elucidates the interactions between lithium polysulfides (LiPSs) and the Ti2-xZnxCS2 surface, as well as the delithiation process of Li2S on the Ti2-xZnxCS2 surface using spin-polarized density functional theory (DFT) calculations. The results demonstrate the importance of surface chemistry and electronic structure of MXenes in LiPSs' adsorption and catalysis capability, providing insights for the preparation and practical application of MXenes in Li-S batteries.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Mingyang Wang, Jianjun Mao, Yudong Pang, Xilin Zhang, Zongxian Yang, Zhansheng Lu, Shuting Yang
Summary: This article systematically investigates the anchoring and electrochemical performance of transition metal carbides as cathode materials for Li-S batteries. The study finds that the non-polar surfaces of these carbides can provide moderate binding strength with LiPS intermediates and facilitate lithium diffusion, while also accelerating sulfur reduction and utilization.
Article
Physics, Applied
Yudong Pang, Xilin Zhang, Mingyang Wang, Zhenpu Shi, Zongxian Yang, Zhansheng Lu, Ruqian Wu
Summary: This study introduces a descriptor (ε(α)) to efficiently identify high-performance electrode materials and reveals a robust linear relationship between the descriptor and adsorption energy. This finding serves as a practical guide for designing high-capacity battery materials and promotes future advancements in this field.
APPLIED PHYSICS LETTERS
(2023)
Article
Chemistry, Physical
Huiyong Wang, Qiang Wan, Zhansheng Lu, Yanlei Wang, Gaopeng Jiang, Jie Shen, Qiaochu Zeng, Suojiang Zhang, Zhongwei Chen, Jianji Wang
Summary: The study presents a novel strategy of bilayer-favored intercalation induced liquid phase exfoliation of bilayer graphene (BLG) under mild conditions. The obtained BLG has high yield, selectivity, structural integrity, low surface oxidation, and great electron mobility. The strategy shows great potential for industrial scale production of high-quality BLG.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Chemistry, Physical
Peng Lv, Donghai Wu, Bingling He, Xue Li, Rui Zhu, Gang Tang, Zhansheng Lu, Dongwei Ma, Yu Jia
Summary: This study proposes an efficient strategy to screen multifunctional electrocatalysts that can simultaneously reduce all NOx species. By using the first-principles method and taking double-atom catalysts embedded N-doped graphene as examples, the proposed strategy is proven to be effective, and Cu-2@NG is identified as the best catalyst.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Chemistry, Multidisciplinary
Yuanyuan Wang, Mengru Wang, Zhansheng Lu, Dongwei Ma, Yu Jia
Summary: This study proposes a strategy to realize multifunctional single-atom catalysts by introducing new active sites on the surface, achieving efficient oxygen evolution and reduction reactions. By supporting Co single atoms on 1T'-MoS2, promising efficient trifunctional SACs were designed.
Article
Chemistry, Physical
Bingling He, Jiansheng Shen, Bin Wang, Zhansheng Lu, Dongwei Ma
Summary: The study investigates the electrocatalytic hydrogen evolution reaction (HER) over single-atom catalysts based on low-cost TiN through a systematic theoretical approach. Results show that single atoms stabilized by surface vacancies exhibit strong hydrogen binding and high HER catalytic activity.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Physics, Multidisciplinary
Tinggui Chen, Baizhan Xia, Dejie Yu, Chuanxing Bi
Summary: This study proposes a gradient phononic crystal structure for enhanced acoustic sensing. By breaking the symmetry of the PC structure, topologically protected edge states are introduced, resulting in topological acoustic rainbow trapping. The robustness and enhancement properties are verified numerically and experimentally.
