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Science China Chemistry 2017年第8期60卷 1115-1129页

作者： Xian chen Tianmin Wu zhe-ning chen Tan Jin Wei Zhuang Yisong zheng State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matte~ Chinese Academy of Sciences Fuzhou 350002. China

We review in this article our recent simulation works on modeling peptide T-jump and thermal unfolding Fourier transform infrared spectroscopy(FTIR) and two-dimensional infrared(2DIR) spectra. The theoretical and computational techniques used,including Markov state model(MSM), integrated tempering sampling(ITS) and nonlinear exciton propagation(NEP), are first briefly introduced. The protocols for simulating the thermal unfolding as well as T-jump unfolding are then summarized in details. The simulated spectral features, such as the intensity and ellipticity, are demonstrated to agree well with the experimental observations.

关键词： polypeptides amide vibration nonlinear response MSMs T-jump implicit solvent model ITS 2DIR folding landscape

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Toward accurate and efficient dynamic computational strategy for heterogeneous catalysis:Temperature-dependent thermodynamics and kinetics for the chemisorbed on-surface CO

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Chinese Chemical Letters 2022年第11期33卷 4936-4942页

作者： Jun chen Tan Jin Yihuang Jiang Tonghao Shen Mingjun Yang zhe-ning chen Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China State Key Laboratory of Physical Chemistry of Solid Surfaces Fujian Provincial Key Laboratory of Theoretical and Computational ChemistryXiamen UniversityXiamen 361005China University of Chinese Academy of Sciences Beijing 100049China MOE Key Laboratory of Computational Physical Sciences Department of ChemistryFudan UniversityShanghai 200433China Shenzhen Jingtai Technology Co. Ltd.(XtalPi)Fubao CommunityShenzhen 518045China

Computational tools on top of first principle calculations have played an indispensable role in revealing the molecular details,thermodynamics,and kinetics in catalytic *** we proposed a highly efficient dynamic strategy for the calculation of thermodynamic and kinetic properties in heterogeneous catalysis on the basis of efficient potential energy surface(PES)and MD *** CO adsorbate on Ru(0001)surface as the illustrative model system,we demonstrated the PES-based MD can efficiently generate reliable two-dimensional potential-of-mean-force(PMF)surfaces in a wide range of temperatures,and thus temperature-dependent thermodynamic properties can be obtained in a comprehensive investigation on the whole PMF ***,MD offers an effective way to describe the surface kinetics such as adsorbate on-surface movement,which goes beyond the most popular static approach based on free energy barrier and transition state theory(TST).We further revealed that the dynamic strategy significantly improves the predictions of both thermodynamic and kinetic properties as compared to the popular ideal statistic mechanics approaches such as harmonic analysis and *** is expected that this accurate yet efficient dynamic strategy can be powerful in understanding mechanisms and reactivity of a catalytic surface system,and further guides the rational design of heterogeneous catalysts.

关键词： Dynamic strategy Temperature-dependent thermodynamics Statistical sampling Neural networks potential energy surface Operando simulation

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Theoretical Studies on Dehydrogenation Reactions in Mg2（BH4）2（NH2）2 Compounds

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Chinese Journal of Chemical Physics 2012年第6期25卷 676-680,I0003页

作者： zheng chen zhe-ning chen An-an Wu Guo-tao Wu Zhi-tao Xiong Ping chen Xin Xu State Key Laboratory for Physical Chemistry of Solid Surface Fujian Provincial Key Laboratoryof Theoretical and Computational Chemist04 College of Chemistry and Chemical Engineering XiamenUniversity Xiamen 361005 China Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China MOE Laboratory for Computational Physical Science Shanghai Key Laboratory of Molecular Catalysisand Innovative Materials Department of Chemistry Center of Chemistry for Energy Materials FudanUniversity Shanghai 200433 China

Borohydrides have been recently hightlighted as prospective new materials due to their high gravimetric capacities for hydrogen storage. It is, therefore, important to under- stand the underlying dehydrogenation mechanisms for further development of these ma- terials. We present a systematic theoretical investigation on the dehydrogenation mecha- nisms of the Mg2（BH4）2（NH2）2 compounds. We found that dehydrogenation takes place most likely via the intermolecular process, which is favorable both kinetically and thermo- dynamically in comparison with that of the intramolecular process. The dehydrogenation of Mg2（BH4）2（NH2）2 initially takes place via the direct combination of the hydridie H in BH4 and the protie H in NH2-, followed by the formation of Mg-H and subsequent ionic recombination of Mg-Hδ-…Hδ＋-N.

关键词： Hydrogen storage Density functional theory Metal borohydride

Tunable CO_(2)enrichment on functionalized Au surface for enhanced CO_(2)electroreduction

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Nano Research 2023年第4期16卷 4723-4728页

作者： Huimin Wang Yuqing Fu zhe-ning chen Wei Zhuang Minna Cao Rong Cao State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China University of Chinese Academy of Sciences Beijing 100049China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China

Electrochemical conversion of carbon dioxide(CO_(2))to higher-value products provides a forward-looking way to solve the problems of environmental pollution and energy ***,the low solubility of CO_(2)in aqueous electrolytes,sluggish kinetics,and low selectivity hamper the efficient conversion of CO_(2).Here,we report a Au-based hybrid nanomaterial by modifying Au nanoparticles(NPs)with the macrocyclic molecule cucurbit[6]uril(Au@CB[6]).Au@CB[6]displays the optimal selectivity of CO,with the highest CO Faraday efficiency(FECO)reaching 99.50%at−0.6 V *** hydrogen electrode(RHE).The partial current density of CO formed by Au@CB[6]increases dramatically,as 3.18 mA/cm2 at−0.6 V,which is more than ten times as that of oleylamine-coated Au NPs(Au@OAm,0.31 mA/cm2).Operando electrochemical measurement combined with density functional theory(DFT)calculations reveals that CB[6]can gather CO_(2)and lead the increased local CO_(2)concentration near metal interface,which realizes significantly enhanced electrochemical CO_(2)reduction reaction(CO_(2)RR)performance.

关键词： molecular surface functionalization Au nanoparticles macrocyclic molecule tunable CO_(2)enrichment electrochemical CO_(2)reduction reaction

Paired-Pd(Ⅱ) centers embedded in HKUST-1 framework: Tuning the selectivity from dimethyl carbonate to dimethyl oxalate

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Journal of Energy Chemistry 2022年第4期31卷 233-240页

作者： Hong-Zi Tan zhe-ning chen Kai-Qiang Jing Jing Sun Yu-Ping Xu ning-ning Zhang Zhong-ning Xu Guo-Cong Guo State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002FujianChina School of Chemistry&Chemical Engineering Shandong University of TechnologyZibo 255049ShandongChina School of Chemistry and Chemical Engineering Liaocheng UniversityLiaocheng 252000ShandongChina

CO oxidative coupling to dimethyl oxalate(DMO) is the most crucial step in coal to ethylene glycol. Pdbased supported catalysts have been verified effective for generating DMO, but concomitant generation of dimethyl carbonate(DMC) is always unavoidable. It is generally accepted that Pd(0) is the active species for producing DMO, while Pd(II) for DMC. However, density functional theory calculations have proposed that the selectivity to DMO or DMC highly depends on the space state of Pd species rather than its oxidative state. It is thus urgently desired to develop high-efficient catalysts with well-defined structure,and further to elucidate the structure-performance relationship. In this work, HKUST-1 with unique structure of paired-Cu(Ⅱ) centers was chosen as ideal support to construct the catalysts with respective paired-Pd(Ⅱ) centers and isolated-Pd(Ⅱ) centers via in situ Pd species doping. In despite of featuring Pdδ+(δ≈2) oxidation state, the synthesized paired-Pd(Ⅱ)/HKUST-1 catalyst still exhibited DMO as dominant product(90.8% of DMO selectivity). For isolated-Pd(Ⅱ)/HKUST-1 catalyst, however, the main product was DMC(84.8% of DMC selectivity). Based on catalyst characterizations, the structures of paired-Pd(Ⅱ) centers and isolated-Pd(Ⅱ) centers were determined. DMO was generated from the coupling of adjacent *COOCH;intermediates adsorbed on paired-Pd(Ⅱ) centers, while DMC was produced from the reaction between methyl nitrite and the *COOCH;intermediates formed on isolated-Pd(Ⅱ) centers. Current work is the first MOFs-based catalyst with well-defined structure being applied in CO oxidative coupling reaction, which not only sheds light on the structure-performance relationship, but also inspires the potential of using MOFs as tunable platform to design high-efficient catalysts in heterogeneous catalysis.

关键词： CO Methyl nitrite Oxidative coupling Dimethyl oxalate Paired-Pd(Ⅱ)centers HKUST-1

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Sub-10-nm-sized Au@AuxIr1-x metal-core/alloy-shell nanoparticles as highly durable catalysts for acidic water splitting

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National Science Review 2024年第4期11卷 130-140页

作者： Huimin Wang zhe-ning chen Yuanyuan Wang Dongshuang Wu Minna Cao Fanfei Sun Rong Cao State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences University of Chinese Academy of Sciences School of Materials Science and Engineering Nanyang Technological University Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied Physics Chinese Academy of Sciences Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China

The absence of efficient and durable catalysts for oxygen evolution reaction（OER） is the main obstacle to hydrogen production through water splitting in an acidic ele ***,we report a controllable synthesis method of surface IrOxwith changing Au/Ir compositions by constructing a range of sub-10-nm-sized core-shell nanocatalysts composed of an Au core and AuxIr1-xalloy *** particular,Au@Au0.43Ir0.57exhibits 4.5 times higher intrinsic OER activity than that of the commercial Ir/*** X-ray-based spectroscopies,electron microscopy and density functional theory calculations revealed a balanced binding of reaction intermediates with enhanced *** water-splitting cell using a load of 0.02 mgIr/cm2of Au@Au0.43Ir0.57as both anode and cathode can reach 10 mA/cm2at 1.52 V and maintain activity for at least194 h,which is better than the cell using the commercial couple Ir/C‖Pt/C（1.63 V,0.2 h）.

关键词： controllable synthesis of surface IrOx oxygen evolution reaction acidic water splitting catalytic stability transition metal catalysts

Phosphine-Built-In Porous Organic Cage Supported Ultrafine Pd Nanoclusters Enable Highly Efficient and Regioselective Hydrogenation of Epoxides

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CCS Chemistry 2024年第10期6卷 2476-2488页

作者： Xin Zhou Zhaozhan Wang zhe-ning chen Yong Yang CAS Key Laboratory of Bio-Based Materials Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101 Shandong Energy Institute Qingdao 266101 College of Environment and Safety Engineering Qingdao University of Science and TechnologyQingdao 266101 State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002 University of Chinese Academy of Sciences Beijing 100049 Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry Xiamen UniversityXiamen 361005

Selective hydrogenation of epoxides has been regarded as an atom-economical and straightforward method for the synthesis of ***,it remains a big challenge in the precise control of *** date,the reaction enabled by a reusable and high-performance heterogeneous catalyst with excellent regioselectivity is very ***,we develop highly loaded and ultrafine Pd nanoclusters(NCs)encapsulated on a phosphinebuilt-in porous organic cage(FPPOC)for the catalytic hydrogenation of epoxides by molecular *** from the unique characters of uniform dispersion and strong interaction between Pd NCs and FPPOC,the resultant Pd NCs exhibited superior catalytic activity and excellent regioselectivity for the hydrogenation of epoxides under milder conditions.A diverse set of terminal and internal epoxides was efficiently reduced to the corresponding linear or branched alcohols in an extremely regioselective manner,well tolerating diverse functional ***,the catalyst demonstrates high stability and could be reused up to 10 times with marginal decay in activity and ***,the catalyst is applicable for scale-up synthesis with a record turnover number as high as 16,111,to the best of our knowledge,outperforming those previous state-of-the-art *** experiments and characterizations in combination with density functional theory calculations provide insight into the superior activity and excellent regioselectivity.

关键词： porous organic cage phosphine-built-in palladium nanoclusters regioselective hydrogenation epoxides

Accurate Description of Catalytic Selectivity:Challenges and Opportunities for the Development of Density Functional Approximations

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CCS Chemistry 2021年第11期3卷 136-143页

作者： zhe-ning chen Tonghao Shen Yizhen Wang Igor Ying Zhang Collaborative Innovation Center of Chemistry for Energy Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsMOE Key Laboratory of Computational Physical SciencesShanghai Key Laboratory of Bioactive Small MoleculesDepartment of ChemistryFudan UniversityShanghai 200433 State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002

An accurate description of catalytic selectivity poses an enormous challenge for theoretical *** to the absence of a well-defined benchmark set on the catalytic selectivity,the performance of even the widely used density functional approximations(DFAs)is yet to be *** work reports a test set based on the selective hydrogenation ofα,β-unsaturated aldehydes catalyzed by ruthenium(Ru)hydride *** attention is paid to benchmark the regioselectivity of aldehydes to either unsaturated alcohols or saturated *** reference data were calculated by the massive parallel implementation of the coupled-cluster single,double,and perturbative triple excitations[CCSD(T)]approach,based completely on set ***,we performed the microkinetic simulation based on the CCSD(T)energy profiles,serving the most direct criteria for the performance of DFAs on catalytic selectivity of hydrogenation *** this test set,we uncovered the intrinsic difficulty of semilocal and hybrid functionals for such a *** the context of the XYG3-type double hybrid(xDH)framework,we showed that this particular challenge could be addressed by the top rung functionals only when the many-body nondynamic correlation effect was accounted for adequately.A recently proposed xDH,namely scsRPA,showed unprecedented accuracy with only 5%error on *** predicted kinetic selectivity by scsRPA is in close agreement with the reference value,revealing a unique versatility of the top rung DFAs for a reliable description of catalytic selectivity of hydrogenation reactions.

关键词： density functional theory catalytic selectivity doubly hybrid approximation nondynamic correlation

Activating Ru in the pyramidal sites of Ru_(2)P-type structures with earth-abundant transition metals for achieving extremely high HER activity while minimizing noble metal content

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Carbon Energy 2024年第9期6卷 80-92页

作者： Sayed M.El-Refaei Patrícia A.Russo Thorsten Schultz zhe-ning chen Patrick Amsalem Norbert Koch Nicola Pinna Department of Chemistry and the Center for the Science of Materials Berlin Humboldt-Universität zu BerlinBerlinGermany Max-Planck-Institut für Chemische Energiekonversion Mülheim an der RuhrGermany Institut für Physik and Center for the Science of Materials Berlin Humboldt-Universität zu BerlinBerlinGermany Helmholtz-Zentrum Berlin für Materialien und Energie GmbH BerlinGermany State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouChina

Rational design of efficient pH-universal hydrogen evolution reaction catalysts to enable large-scale hydrogen production via electrochemical water splitting is of great significance,yet a challenging ***,Ru atoms in the Ru_(2)P structure were replaced with M=Co,Ni,or Mo to produce M_(2-x)Ru_(x)P *** metals show strong site preference,with Co and Ni occupying the tetrahedral sites and Ru the square pyramidal sites of the CoRuP and NiRuP Ru_(2)P-type *** presence of Co or Ni in the tetrahedral sites leads to charge redistribution for Ru and,according to density functional theory calculations,a significant increase in the Ru d-band *** a result,the intrinsic activity of CoRuP and NiRuP increases considerably compared to Ru_(2)P in both acidic and alkaline *** effect is not observed for MoRuP,in which Mo prefers to occupy the pyramidal *** particular,CoRuP shows state-of-the-art activity,outperforming Ru_(2)P with Pt-like activity in 0.5 M H_(2)SO_(4)(η_(10)=12.3 mV;η100=52 mV;turnover frequency(TOF)=4.7 s^(-1)).It remains extraordinarily active in alkaline conditions(η10=12.9 mV;η_(100)=43.5 mV)with a TOF of 4.5 s^(-1),which is 4x higher than that of Ru_(2)P and 10x that of Pt/*** increase in the Co content does not lead to drastic loss of activity,especially in alkaline medium,where,for example,the TOF of Co_(1.9)Ru_(0.1)P remains comparable to that of Ru_(2)P and higher than that of Pt/C,highlighting the viability of the adopted approach to prepare cost-efficient catalysts.

关键词： electrocatalysis ruthenium phosphide transition metal phosphonates

Rational Preparation of Atomically Precise Non-Alkyl Tin-Oxo Clusters with Theoretical to Experimental Insights into Electrocatalytic CO_(2)Reduction Applications

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CCS Chemistry 2021年第10期3卷 2607-2616页

作者： Di Wang zhe-ning chen Qing-Rong Ding cheng-cheng Feng San-Tai Wang Wei Zhuang Lei Zhang State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002 University of Chinese Academy of Sciences Beijing 100049

Tin oxides(SnO_(2))have been widely utilized in electronics,nanolithography,and *** the atomically precise models of SnO_(2),tin-oxo clusters(TOCs)not only provide opportunities for mechanism studies,but they also extend potential applications through structural ***,to date,most of the reported TOCs belong to alkyl organotin complexes,which are usually toxic to the human body and the active sites are difficult to expose for catalysis.

关键词： cluster compounds tin oxides atomic structure green synthesis electrocatalytic CO_(2)red uction