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中国化学快报:英文版 2023年第8期34卷 328-332页

作者： Chaozheng He Yue Yu Chenxu Zhao Jinrong Huo Institute of Environmental and Energy Catalysis School of Materials Science and Chemical EngineeringXi’an Technological UniversityXi’an 710021China School of Sciences Xi’an Technological UniversityXi’an 710021China

Hydrocarbons are promising products for CO_(2)electroreduction(CRR)while is impeded by the low selectivity.Turning the curvature of the active site is an effective strategy to change the adsorption properties and further regulate the product distribution and reactivity.Herein,we have designed a novel V single atom catalyst(SAC)based on rolled two-dimensional(2D)BC_(3)N_(2)substrate with different curvatures.The results have demonstrated that increased curvature can enhance the adsorption strength of CRR intermediates,which follows different mechanisms for systems with low and high curvature.This character eventually leads to the deviation away from the scaling line between Ead[CO]∼Ead[COOH]based on transition metals for V@2D-BC_(3)N_(2)systems.3-3 system is screened as the optimal candidate for hydrocarbons production due to the enhanced binding ability of adsorbates,which can increase the reactivity for hydrocarbons production and hinder the production of H2 and HCOOH simultaneously.

关键词： V doped 2D BC_(3)N_(2) Curvature effect CO_(2)electroreduction Hydrocarbons production d-band center theory Geometric and electronic properties

Computational design of BC_(3)N_(2) based single atom catalyst for dramatic activation of inert CO_(2) and CH4 gasses into CH_(3)COOH with ultralow CH_(4) dissociation barrier

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Chinese Chemical Letters 2023年第1期34卷 493-498页

作者： Chenxu Zhao Menghui Xi Jinrong Huo Chaozheng He Ling Fu Institute of Environment and Energy Catalysis School of Materials Science and Chemical EngineeringXi’an Technological UniversityXi’an 710021China School of Sciences Xi’an Technological UniversityXi’an 710021China College of Resources and Environmental Engineering Tianshui Normal UniversityTianshui 741001China

The production of CH_(3)COOH from CO_(2)and CH_(4) has stimulated much interest due to the high energy density of C2 species.Various kinds of catalysts have been developed while the high dissociation barrier of CH_(4) and low selectivity still hinders the efficiency of the reaction.We have herein proposed a novel catalyst with single metals loaded on 2D BC_(3)N_(2) substrate(M@2D-BC_(3)N_(2))based on density functional theory.Among numerous candidates,Pt@2D-BC_(3)N_(2) possesses the most favorable reactivity with an ultralow barrier of CH_(4) splitting(0.26 e V),which is due to the efficient capture ability of CH_(4) on Pt site.Besides,the selectivity for CH_(3)COOH is also very high,which mainly stems from the unique electronic properties of molecules and substrate:The degenerated states,including s,px,pyand pz,in CO_(2)reflects the existence of delocalizedπbonds between C and O.This can interact with states of Pt(s),Pt(pz),Pt(dxz),Pt(dyz),and Pt(z2)in Pt@2D-BC_(3)N_(2).The kinetics model also proves that our system can promote CH_(3)COOH production via simply increasing the temperature or the coverage of CH_(4) and CO_(2).Our results provide a reasonable illustration in clarifying mechanism and propose promising candidates with high reactivity for further study.

关键词： Density functional theory CO_(2)/CH4 coactivation 2D BC_(3)N_(2)substrate CH_(3)COOH production

Associative vs. dissociative mechanism: Electrocatalysis of nitric oxide to ammonia

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Chinese Chemical Letters 2022年第2期33卷 1051-1057页

作者： Chaozheng He Jia Wang Ling Fu Chenxu Zhao Jinrong Huo Institute of Environment and Energy Catalysis Shaanxi Key Laboratory of Optoelectronic Functional Materials and DevicesSchool of Materials Science and Chemical EngineeringXi’an Technological UniversityXi’an 710021China College of Resources and Environmental Engineering Tianshui Normal UniversityTianshui 741001China School of Sciences Xi’an Technological UniversityXi’an 710021China

Nitric oxide reduction to ammonia by electrocatalysis is the potential application in the elimination of smog and energy conversion. In this work, the feasibility of the application of two-dimensional metal borides(MBenes) in nitric oxide electroreduction reaction(NOER) was investigated through density functional theory calculations. Including the geometry and electronic structure of five kinds of MBenes, the adsorption of NO on the surface of these substrates, the selective adsorption of hydrogen protons during the hydrogenation process, and the overpotential in the electrocatalytic ammonia synthesis process. As a result, Mn B exhibited the most favorable catalytic performance according to the associative pathways,which is thermodynamically performed spontaneously, and WB has a minimum overpotential of 0.37 V vs. RHE in the process of ammonia production according to the dissociative pathway. Overall, our work is the first to explore the electrocatalytic NO through the dissociative mechanism to synthesize ammonia in-depth and proves that MBenes are efficient NO electrocatalytic ammonia synthesis catalysts. These research results provide a new direction for the development of electrocatalytic ammonia synthesis experimentally and theoretically.

关键词： MBenes Nitric oxide NOER First-principles calculation Ammonia

Highly active Fe_(36)Co_(44) bimetallic nanoclusters catalysts for hydrolysis of ammonia borane: The first-principles study

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Chinese Chemical Letters 2023年第2期34卷 550-556页

作者： Jinrong Huo Haocong Wei Ling Fu Chenxu Zhao Chaozheng He School of Sciences Xi'an Technological UniversityXi'an 710021China Shaanxi Key Laboratory of Optoelectronic Functional Materials and Devices School of Materials Science and Chemical EngineeringXi'an Technological UniversityXi'an 710021China Institute of Environmental and Energy Catalysis School of Materials Science and Chemical EngineeringXi'an Technological UniversityXi'an 710021China College of Resources and Environmental Engineering Tianshui Normal UniversityTianshui 741001China

In this paper,Fe_(36)Co_(44)nanocluster structure is used to catalyze the hydrolysis reaction of ammonia borane to produce H_(2).Firstly,we complete the construction of Fe_(36)Co_(44)cluster structure and calculate the electronic properties of the cluster.By comparing the adsorption process of Ammonia Borane (AB) in active sites of the cluster,which have different Effective Coordination Number (ECN),the qualitative relationship between ECN and the catalytic activation of AB is clarified,and the optimal catalytic active site is obtained.Then,from the perspective of different reaction paths,we study the hydrolysis reaction of AB in multiple paths,and obtain 5 different reaction paths and energy profiles.The calculation results show that in the case of N–H bond priority break (path 5),the reaction has the minimum rate-determining step (RDS) barrier (about 1.02 e V) and the entire reaction is exothermic (about 0.40 e V).So,path 5 is an optimal catalytic reaction path.This study will have an important guiding significance for the study of the AB hydrolysis reaction mechanism.

关键词： The first-principles NH_(3)BH_(3) Hydrolysis reaction FeCo cluster Catalyst

CO adsorption on metal doped 2D InSe:Mechanism and application

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Progress in Natural Science:Materials International 2019年第3期29卷 305-309页

作者： Chenxu Zhao Wang Gao Qing Jiang Key Laboratory of Automobile Materials Ministry of EducationDepartment of Materials Science and EngineeringJilin University

A novel-type material based on metal doped 2D InSe (M@2DInSe) has been proposed for CO sensing.The results reveal that the conventional Blyholder mechanism can be applicable to M@2DInSe systems,and the charge transfer between CO and M@2DInSe can serve as an effective measurement for the adsorption energy of CO.In M@2DInSe,the response of electronic structures towards CO adsorption is also strongly correlated with the adsorption energy of CO,demonstrating an apparent metal-to-insulator transition for Fe@2DInSe and Mo@2DInSe under the influence of CO adsorption.These findings provide a new material-design scheme to detect CO molecules and promising candidates for further experimental studies.

关键词： Se CO adsorption on metal doped 2D InSe:Mechanism and application

Hydrogen generation of ammonia borane hydrolysis catalyzed by Fe_(22)@Co_(58) core-shell structure

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Chinese Chemical Letters 2021年第7期32卷 2269-2273页

作者： Jinrong Huo Ling Fu Chenxu Zhao Chaozheng He School of Sciences Xi'an Technological UniversityXi'an 710021China Shaanxi Key Laboratory of Optoelectronic Functional Materials and Devices School of Materials Science and Chemical EngineeringXi'an Technological UniversityXi'an 710021China Institute of Environmental and Energy Catalysis School of Materials Science and Chemical EngineeringXi'an Technological University.Xi'an 710021China College of Resources and Environmental Engineering Tianshui Normal UniversityTianshui 741001China

In this paper,the process of ammonia borane(AB)hydrolysis generate H_(2) on the transition metal Fe@Co core-shell structure has been obtained.According to the different roles played by H_(2)O molecules and the number of H_(2)O molecules involved,there are three schemes of reaction paths.RouteⅠdoes not involve the dissociation of H_(2)O molecules and all H atoms come from AB.Moreover,the H_(2)O molecule has no effect on the breaking of the B—H bond or the N—H bond.The reaction absorbs more heat during the formation of the second and third H_(2) molecules.RouteⅡincludes the dissociation of H_(2)O molecules and the cleavage of B—H or N—H bonds,respectively,and the reaction shows a slight exotherm.RouteⅢstarted from the break of the B—N bond and obtained 3H_(2) molecules through the participation of different numbers of H_(2)O molecules.After multiple comparative analyses,the optimal hydrolysis reaction path has been obtained,and the reaction process can proceed spontaneously at room temperature.

关键词： Fe_(22)@Co_(58)core-shell Hydrolysis reaction Catalyst Ammonia borane Hydrogen generation

Rich B active centers in Penta-B_(2)C as high-performance photocatalyst for nitrogen reduction

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Chinese Chemical Letters 2021年第12期32卷 3821-3824页

作者： Ran Wang Chaozheng He Weixing Chen Chenxu Zhao Jinrong Huo Institute of Environmental and Energy Catalysis School of Materials Science and Chemical EngineeringXi'an Technological UniversityXi'an 710021China Shaanxi Key Laboratory of Optoelectronic Functional Materials and Devices School of Materials Science and Chemical EngineeringXi'an Technological UniversityXi'an 710021China School of Sciences Xi'an Technological UniversityXi'an 710021China

The photocatalytic nitrogen reduction reaction(NRR) has mild reaction conditions and only requires sunlight energy as a driving force to replace the traditional ammonia synthesis method. We herein investigate the catalytic activity and selectivity on Penta-B_(2)C for NRR by using density functional theory calculations. Penta-B_(2)C is a semiconductor with an indirect bandgap(2.328 e V) and is kinetically stable based on molecular dynamic simulations. The optical absorption spectrum of Penta-B;C is achieved in the ultraviolet and visible range. Effective light absorption is more conducive to generate photo-excited electrons and improving photocatalytic performances. Rich B atoms as activation sites in Penta-B_(2)C facilitate capturing N_(2). The activated N_(2)molecule prefers the side-on adsorption configuration on Penta-B_(2)C, which facilitates the subsequent reduction reaction. Among considered NRR mechanisms on Penta-B_(2)C, the best pathway prefers the enzymatic mechanism, only required a low onset potential of 0.23 V. The hydrogen evolution reaction is inhibited when the hydrogen adsorption concentration is increased or N_(2)molecules first occupy the adsorption sites. Our results indicate Penta-B_(2)C is a highly reactive and selective photocatalyst for NRR. Our work provides theoretical insights into the experiments and has guiding significance to synthesize efficient NRR photocatalysts.

关键词： Nitrogen reduction Photocatalytic Penta-B_(2)C Mechanism B active center

Principles for designing CO_(2) adsorption catalyst: Serving thermal conductivity as the determinant for reactivity

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Chinese Chemical Letters 2022年第2期33卷 990-994页

作者： Chaozheng He Haotian Wang Ling Fu Jinrong Huo Zhiheng Zheng Chenxu Zhao Meng An Institute of Environmental and Energy Catalysis School of Materials Science and Chemical EngineeringXi’an Technological UniversityXi’an 710021China College of Mechanical and Electrical Engineering Shaanxi University of Science and TechnologyXi’an 710021China School of Sciences Xi’an Technological UniversityXi’an 710021China College of Resources and Environmental Engineering Tianshui Normal UniversityTianshui 741001China School of Energy and Materials Shanghai Polytechnic UniversityShanghai 201209China Shanghai Engineering Research Center of Advanced Thermal Functional Materials Shanghai Polytechnic UniversityShanghai 201209China

CO_(2)is a representative prototype model in energy and environmental fields.Many factors for CO_(2)capture and activation have been investigated extensively but the research on the influence of thermal conductivity is still absence.We herein have calculated many properties,including dipole moment,electric structure,and adsorption energies,on Pt doped graphene and 2D BC_(3)N_(2)substrates and served the thermal conductivity as the bridge.Our results have demonstrated that the lower (higher) thermal conductivity for 2D BC_(3)N_(2)(graphene) corresponds to larger (lower) dipole moment,which is beneficial for CO_(2)activation (capture) process.Our research have not only revealed the dominant role of heat conductivity for CO_(2)capture and activation,but also paved the way for further catalyst design of various areas.

关键词： 2D materials Absorption Thermal conductivity Polarization bonding Molecular dynamics simulations Density functional theory

Defect engineering for high-selection-performance of NO reduction to NH3 over CeO_(2)(111)surface:A DFT study

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Chinese Chemical Letters 2022年第1期33卷 527-532页

作者： Chaozheng He Risheng Sun Ling Fu Jinrong Huo Chenxu Zhao Xiuyuan Li Yan Song Sumin Wang Shaanxi Key Laboratory of Optoelectronic Functional Materials and Devices School of Materials Science and Chemical EngineeringXi'an Technological UniversityXi'an 710021China Institute of Environmental and Energy Catalysis School of Materials Science and Chemical EngineeringXi'an Technological UniversityXi'an 710021China College of Resources and Environmental Engineering Tianshui Normal UniversityTianshui 741001China School of Sciences Xi'an Technological UniversityXi'an 710021China

To reduce the greenhouse effect caused by the surgery of nitrogen-oxides concentration in the atmosphere and develop a future energy carrier of renewables,it is very critical to develop more efficient,controllable,and highly sensitive catalytic materials.In our work,we proposed that nitric oxide(NO),as a supplement to N_(2) for the synthesis of ammonia,which is equipped with a lower barrier.And the study highlighted the potential of CeO_(2)(111)nanosheets with La doping and oxygen vacancy(OV)as a high-performance,controllable material for NO capture at the site of Vo site,and separation the process of hydrogenation.We also reported that the E_(ads) of-1.12 eV with horizontal adsorption and the Bader charge of N increasing of 0.53|e|and O increasing of 0.17|e|at the most active site of reduction-OV predicted.It is worth noting thatΔG of NORR(NO reduction reaction)shows good performance(thermodynamically spontaneous reaction)to synthesize ammonia and water at room temperature in the theoretical calculation.

关键词： La-doping CeO_(2) Bader analysis Oxygen vacancy(OV) Single atom catalysis Synergistic effect NO reduction reaction(NORR)

Identification of niclosamide as a novel antiviral agent against porcine epidemic diarrhea virus infection by targeting viral internalization

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Virologica Sinica 2023年第2期38卷 296-308页

作者： Yue Wang Huimin Huang Dongliang Li Chenxu Zhao Shuai Li Panpan Qin Yaqin Li Xia Yang Wenjuan Du Wentao Li Yongtao Li College of Veterinary Medicine Henan Agricultural UniversityZhengzhou450002China State Key Laboratory of Agricultural Microbiology College of Veterinary MedicineHuazhong Agricultural UniversityWuhan430070China Faculty of Veterinary Medicine Utrecht UniversityUtrecht3584 CLthe Netherlands Hubei Hongshan Laboratory Wuhan430070China

Porcine epidemic diarrhea virus(PEDV),an enteropathogenic coronavirus,has catastrophic impacts on the global pig industry.However,there remain no effective drugs against PEDV infection.In this study,we utilized a recombinant PEDV expressing renilla luciferase(PEDV-Rluc)to screen potential anti-PEDV agents from an FDAapproved drug library in Vero cells.Four compounds were identified that significantly decreased luciferase activity of PEDV-Rluc.Among them,niclosamide was further characterized because it exhibited the most potent antiviral activity with the highest selectivity index.It can efficiently inhibit viral RNA synthesis,protein expression and viral progeny production of classical and variant PEDV strains in a dose-dependent manner.Time of addition assay showed that niclosamide exhibited potent anti-PEDV activity when added simultaneously with or after virus infection.Furthermore,niclosamide significantly inhibited the entry stage of PEDV infection by affecting viral internalization rather than viral attachment to cells.In addition,a combination with other small molecule inhibitors of endosomal acidification enhanced the anti-PEDV effect of niclosamide in vitro.Taken together,these findings suggested that niclosamide is a novel antiviral agent that might provide a basis for the development of novel drug therapies against PEDV and other related pathogenic coronavirus infections.

关键词： Coronavirus Porcine epidemic diarrhea virus(PEDV) Niclosamide(NIC) Antiviral Virus entry Endocytosis Host-targeted antivirals