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Nitric oxide assists nitrogen reduction reaction on 2D MBene: A theoretical study

Chinese Chemical Letters 2024年第5期35卷 428-433页

作者： chaozheng he Jia Wang Ling Fu Wei Wei henan Engineering Center of New Energy Battery Materials College of Chemistry and Chemical EngineeringShangqiu Normal UniversityShangqiu 476000China School of Chemistry and Chemical Engineering Shandong Provincial Key Laboratory/Collaborative Innovation Center of Chemical Energy Storage&Novel Cell TechnologyLiaocheng UniversityLiaocheng 252059China 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

Electrocatalytic synthesis of ammonia as an environment-friendly and sustainable development method has received widespread attention in recent years.Two-dimensional(2D)materials are a promising catalyst for ammonia synthesis due to their large surface area.In this work,we have constructed a series of 2D metal borides(MBenes)with transition metal(TM)defects(TMd-MBenes)and comprehensively calculated the reactivity of electrocatalytic synthesis of ammonia-based on density functional theory.The results have demonstrated that the TMd-MBenes can effectively activate nitrogen oxide(NO)and nitrogen(N2)molecules thermodynamically.Particularly interesting,the co-chemisorption of O atoms,dissociated from NO,can facilitate the spilled of the inert N2 molecules into single N atoms,which can further hydrogenate into ammonia easily with an ultralow limiting potential of 0.59 V on TMd-MnB.Our research has not only provided clues for catalyst design for experimental study but also paved the way for the industrial application of electrocatalytic ammonia synthesis.

关键词： 2D mbenes Nitrogen electro-reduction DFT N_(2)activation Ammonia synthesis

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First-principles study of the relationship between the formation of single atom catalysts and lattice thermal conductivity

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Chinese Chemical Letters 2024年第6期35卷 502-506页

作者： chaozheng he Pei Shi Donglin Pang Zhanying Zhang Long Lin Yingchun Ding Department of Chemistry and Chemical Engineering Liaocheng UniversityLiaocheng 252059China henan Key Laboratory of Materials on Deep-Earth Engineering School of Materials Science and EngineeringHenan Polytechnic UniversityJiaozuo 454000China School of Materials Science and Engineering Henan Polytechnic UniversityJiaozuo 454000China Department of Basic Medicine North Sichuan Medical CollegeNanchong 637000China

Single atom catalysts(SACs)have been in the forefront of catalysts research because of their high efficiency and low cost and provide new ideas for development of renewable energy conversion and storage technologies.However,the relationship between the intrinsic properties of materials such as lattice thermal conductivity and catalysis remains to be explored.In this work,the lattice thermal conductivity of BN and graphene was calculated by Sheng BTE.In addition,the adsorption properties of 3d-TM(TM=V,Cr,Mn,Fe,Co,Ni)on BN and graphene were investigated using first-principles methods,and it was found that Ni atom can form relatively stable SACs compared to other TMs.The molecular dynamics(MD)simulation and migration barrier of Ni loaded on BN and graphene were calculated.Our study found that graphene has higher thermal conductivity and is easier to form SACs than BN,but the SACs formed on BN surface have higher thermodynamic stability.

关键词： First-principles calculation Thermal conductivity Single atom catalysts Graphene BN

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A novel method for atomization energy prediction based on natural-parameter network

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Chinese Chemical Letters 2024年第1期35卷 505-509页

作者： Chaoqin Chu Qinkun Xiao chaozheng he Chen Chen Lu Li Junyan Zhao Jinzhou Zheng Yinhuan Zhang School of Mechanical and Electrical Engineering Xi’an Technological UniversityXi’an 710021China School of Electrical and Information Engineering Xi’an Technological UniversityXi’an 710021China School of Materials Science and Chemical Engineering Xi’an Technological UniversityXi’an 710021China

Atomization energy(AE)is an important indicator for measuring material stability and reactivity,which refers to the energy change when a polyatomic molecule decomposes into its constituent atoms.Predicting AE based on the structural information of molecules has been a focus of researchers,but existing methods have limitations such as being time-consuming or requiring complex preprocessing and large amounts of training data.Deep learning(DL),a new branch of machine learning(ML),has shown promise in learning internal rules and hierarchical representations of sample data,making it a potential solution for AE prediction.To address this problem,we propose a natural-parameter network(NPN)approach for AE prediction.This method establishes a clearer statistical interpretation of the relationship between the network’s output and the given data.We use the Coulomb matrix(CM)method to represent each compound as a structural information matrix.Furthermore,we also designed an end-to-end predictive model.Experimental results demonstrate that our method achieves excellent performance on the QM7 and BC2P datasets,and the mean absolute error(MAE)obtained on the QM7 test set ranges from 0.2 kcal/mol to 3 kcal/mol.The optimal result of our method is approximately an order of magnitude higher than the accuracy of 3 kcal/mol in published works.Additionally,our approach significantly accelerates the prediction time.Overall,this study presents a promising approach to accelerate the process of predicting structures using DL,and provides a valuable contribution to the field of chemical energy prediction.

关键词： Structure prediction Atomization energy Deep learning Coulomb matrix NPN End-to-end

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A promising controllable CO_(2)capture and separation materials for CO_(2)/CH_(4)/H_(2)under electric field

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Chinese Chemical Letters 2023年第5期34卷 587-593页

作者： chaozheng he Houyong Yang Ling Fu Shaanxi Key Laboratory of Optoelectronic Functional Materials and Devices Institute of Environment and Energy CatalysisSchool of Materials Science and Chemical EngineeringXi'an Technological UniversityXi'an 710021China College of Resources and Environmental Engineering Tianshui Normal UniversityTianshui 741001China

As the greenhouse effect concerns increases,the development of new materials for the efficient capture and separation of CO_(2)gas from gas mixtures has become a matter of urgency.In this study,we performed density functional theory(DFT)calculations to investigate the adsorption and separation behavior of CO_(2)/CH_(4)/H_(2)on the surface of two-dimensional(2D)Al_(2)C materials under positive/negative applied electric fields.In the absence of an electric field CO_(2)is weakly physisorbed on the Al_(2)C surface,but with the application of an applied electric field,the adsorption state of CO_(2)gradually changes from physical to chemisorption(adsorption energy changes from-0.29 e V to-3.61 e V),while the negative electric field has little effect on the adsorption of CO_(2).We conclude that the C=O bond in adsorbed CO_(2)can be activated under an external electric field(maximum activation of 15%under an external electric field of 0-0.005 a.u.).Only in the presence of an applied electric field of 0.0033 a.***.and temperatures above525 K/675 K can the adsorption/separation reaction of CO_(2)single adsorption and CO_(2)/CH_(4)/H_(2)mixture be spontaneous.The adsorption/desorption of CO_(2)on Al_(2)C nanosheet in an electric field of 0.003-0.0033 a.***.is all exothermic,which can be easily controlled by switching on/off the electric field without any energy barriers.The capacity of Al_(2)C to capture CO_(2)per unit electric field decreases with increasing CO_(2)concentration,but still has efficient gas separation properties for CO_(2)/CH_(4)/H_(2).Our theoretical results could provide guidance for designing high-capacity and high-selectivity CO_(2)capture materials.

关键词： CO_(2)capture Electric-field controlled CO_(2)/CH_(4)/H_(2)mixture sequestration Density functional theory Two-dimensional materials

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An efficient single atom catalysts Os/P_(3)C sheet for ammonia borane dehydrogenation

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Chinese Chemical Letters 2022年第6期33卷 3281-3286页

作者： chaozheng he Quan Zhang Jinrong Huo Ling Fu Shaanxi Key Laboratory of Optoelectronic Functional Materials and Devices School of Materials Science and Chemical EngineeringInstitute of Environment and Energy CatalysisXi’an Technological UniversityXi’an 710021China School of Sciences Xi’an Technological UniversityXi’an 710021China College of Resources and Environmental Engineering Tianshui Normal UniversityTianshui 741001China

Ammonia borane(NH_(3)BH_(3),AB)has been considered to be a promising chemical hydrogen storage material.Based on density functional theory,a series of transition metal atoms supported P_(3)C(P_(3)C_O)sheet is systematically investigated to screen out the most promising catalyst for dehydrogenation of AB.The results indicate that the Os/P_(3)C and Os/P_(3)C_O could be an efficient single atom catalyst(SACs)and the stepwise reaction pathway with free energy barrier of 2.07 and 1.54 e V respectively.Remarkably,the rate constant further quantitatively confirmed the real situation of the first step of dehydrogenation of AB on the Os/P_(3)C and Os/P_(3)C_O substrates.We found that k_(f1)at 400 K is equivalent to k_(f2)at 800 K,which greatly improves the temperature of the first step of AB dehydrogenation on P_(3)C_O.We hope this work can provide a promising method for the design of catalysts for AB dehydrogenation reactions on the surface of two-dimensional materials(2D).

关键词： Ammonia borane Two-dimensional materials Dehydrogenation Single atom catalyst Microkinetic model

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Turning the V site in V@2D-BC_(3)N_(2)complex to high curvature state for efficient CO_(2)electroreduction to hydrocarbons

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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

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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

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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

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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

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A DFT study of two-dimensional P_2Si monolayer modified by single transition metal(Sc-Cu)atoms for efficient electrocatalytic CO_(2)reduction

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Chinese Chemical Letters 2023年第5期34卷 580-586页

作者： chaozheng he Houyong Yang Xi Fu Xiaoli Cheng Jiyuan Guo Ling Fu Institute of Environmental 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 Science Hunan University of Science and EngineeringYongzhou 425199China Department of Physics Jishou UniversityJishou 416000China School of Science Jiangsu University of Science and TechnologyZhenjiang 212003China College of Resources and Environmental Engineering Tianshui Normal UniversityTianshui 741001China

In the present work,a stable two-dimensional(2D)P_(2)Si monolayer was predicted.The monolayer is semimetallic/metallic under the PBE/HSE06 functional and is mechanically isotropic.The stability of the P_(2)Si monolayer has been proved via cohesive energy,mechanical criteria,molecular dynamics simulation,and phonon dispersion respectively,and the monolayer possesses high carrier mobility which is three times that of Mo S_(2).On the other hand,the catalytic performance of the P_(2)Si monolayer modified with a single transition metals(M=Sc-Cu)atom for the electrochemical reduction of CO_(2)was investigated,and the monolayer can catalyze CO_(2)with three constraints:stable molecular dynamics,high migration potential of metal atoms,and suitable band gap for electrocatalyst after metal doping exhibiting excellent catalytic stabilization activity and CRR selectivity.In addition,the reduction product of V@P_(2)Si is HCOOH with an overpotential as low as 0.75 V,and the most suitable reaction path is^(*)CO_(2)→^(*)CHOO→O^(*)CHOH→^(*)+HCOOH with the final reduction product HCOOH obtained.As a whole,the above results endow the P_(2)Si monolayer to be a good 2D material holding great promises for applications in nanoelectronics and CO_(2)reduction catalysts.

关键词： First-principles calculation Global optimization method CO_(2)electrochemical reduction reaction Single-atom catalysts Phosphorus silicon compound

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