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Precision Chemistry 2024年第6期2卷 245-255页

作者： Hui Ye Lina Cao Minghui Gu Han Nie Qingqing Gu Bing Yang Yunxing Bai Qinxue Nie Weixin Huang Junling Lu Institute of Advanced Technology Key Laboratory of Precision and Intelligent ChemistryDepartment of Chemical PhysicsHefei National Research Center for Physical Sciences at the MicroscaleKey Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education InstitutesUniversity of Science and Technology of ChinaHefei 230026P.R.China CAS Key Laboratory of science and Technology on Applied catalysis Dalian Institute of Chemical PhysicsThe Chinese Academy of SciencesDalian 116023P.R.China

Propane dehydrogenation(PDH),an atom-economic reaction to produce high-value-added propylene and hydrogen with high efficiency,has recently attracted extensive attention.The severe deactivation of Pt-based catalysts through sintering and coking remains a major challenge in this high-temperature reaction.The introduction of Sn as a promoter has been widely applied to improve the stability and selectivity of the catalysts.However,the selectivity and stability of PtSn catalysts have been found to vary considerably with synthesis methods,and the role of Sn is still far from fully understanding.To gain in-depth insights into this issue,we synthesized a series of PtSn/SiO_(2)and SnPt/SiO_(2)catalysts by varying the deposition sequence and Pt:Sn ratios using atomic layer deposition with precise control.We found that PtSn/SiO_(2)catalysts fabricated by the deposition of SnO_(x)first and then Pt,exhibited much better propylene selectivity and stability than the SnPt/SiO_(2)catalysts synthesized the other way around.We demonstrate that the presence of Sn species at the Pt-SiO_(2)interface is of essential importance for not only the stabilization of PtSn clusters against sintering under reaction conditions but also the promotion of charge transfers to Pt for high selectivity.Besides the above,the precise regulation of the Sn content is also pivotal for high performance,and the excess amount of Sn might generate additional acidic sites,which could decrease the propylene selectivity and lead to heavy coke formation.These findings provide deep insight into the design of highly selective and stable PDH catalysts.

关键词： Propane dehydrogenation PtSn catalysts sintering coke formation acidity

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Polyzwitterionic cross-linked double network hydrogel electrolyte enabling high-stable Zn anode

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Nano Research 2024年第6期17卷 5278-5287页

作者： Mengyu Shi Junlong Zhang Guochuan Tang Ben Wang Sen Wang Xiaoxian Ren Guojie Li Weihua Chen Chuntai Liu Changyu Shen State Key Laboratory of Structural Analysis Optimization and CAE Software for Industrial EquipmentNational Engineering Research Center for Advanced Polymer Processing TechnologyZhengzhou UniversityZhengzhou 450002China College of Chemistry and Green catalysis center Zhengzhou UniversityZhengzhou 450001China Research Institute of Interdisciplinary science and School of Materials science and Engineering Dongguan University of TechnologyDongguan 523808China

Zn metal anode suffers from dendrite issues and passive byproducts,which severely plagues the practical application of aqueous Zn metal batteries.Herein,a polyzwitterionic cross-linked double network hydrogel electrolyte composed of physical crosslinking(hyaluronic acid)and chemical crosslinking(synthetic zwitterionic monomer copolymerized with acrylamide)is introduced to overcome these obstacles.On the one hand,highly hydrophilic physical network provides an energy dissipation channel to buffer stress and builds a H_(2)O-poor interface to avoid side reactions.On the other hand,the charged groups(sulfonic and imidazolyl)in chemical crosslinking structure build anion/cation transport channels to boost ions’kinetics migration and regulate the typical solvent structure[Zn(H_(2)O)_(6)]^(2+)to R-SO_(3)^(−)[Zn(H_(2)O)_(4)]^(2+),with uniform electric field distribution and significant resistance to dendrites and parasitic reactions.Based on the above functions,the symmetric zinc cell exhibits superior cycle stability for more than 420 h at a high current density of 5 mA·cm^(−2),and Zn||MnO_(2)full cell has a reversible specific capacity of 150 mAh·g^(−1)after 1000 cycles at 2 C with this hydrogel electrolyte.Furthermore,the pouch cell delivers impressive flexibility and cyclability for energy-storage applications.

关键词： Zn anode dendrites parasitic reactions polyzwitterion double network hydrogel electrolyte

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Highly selective and efficient photocatalytic NO removal:Charge carrier kinetics and interface molecular process

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Nano Research 2024年第3期17卷 1003-1026页

作者： Huan Shang Hongbao Jia Pengpeng Li Hao Li Wenbin Zhang Shuangjun Li Qing Wang Shuning Xiao Ding Wang Guisheng Li Dieqing Zhang School of Materials and Chemistry University of Shanghai for Science and TechnologyShanghai 200093China The Education Ministry Key Lab of Resource Chemistry Joint International Research Laboratory of Resource Chemistry of Ministry of EducationShanghai Key Laboratory of Rare Earth Functional Materialsand Shanghai Frontiers Science Center of Biomimetic CatalysisShanghai Normal UniversityShanghai 200234China School of Environmental science and Engineering Shanghai Jiao Tong UniversityShanghai 200240China

The widespread nitrogen oxides(NOx,mainly in NO)in the atmosphere have threatened human health and ecological environment.The dilute NO(ppb)is difficult to efficiently remove via the traditional process due to its characteristics of low concentration,wide range,large total amount,etc.Photocatalysis can utilize solar energy to purify NO pollutants under mild conditions,but its application is limited due to the low selectivity of nitrate and poor activity of NO removal.The underlying reason is that the interface mechanism of NO oxidation is not clearly understood,which leads to the inability to accurately regulate the NO oxidation process.Herein,the recent advances in the photocatalytic oxidation of NO are summarized.Firstly,the common strategies to effectively regulate carrier dynamics such as morphology control,facet engineering,defect engineering,plasma coupling,heterojunction and single-atom catalysts are discussed.Secondly,the progress of enhancing the adsorption and activation of reactants such as NO and O_(2) during NO oxidation is described in detail,and the corresponding NO oxidation mechanisms are enumerated.Finally,the challenges and prospects of photocatalytic NO oxidation are presented in term of nanotechnology for air pollution control.This review can shed light on the interface mechanism of NO oxidation and provide illuminating information on designing novel catalysts for efficient NOx control.

关键词： nitrogen oxide(NO)oxidation photocatalysis NO/O_(2)activation charge carrier kinetics interfacial mechanism

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Electronic structure factors and the importance of adsorbate effects in chemisorption on surface alloys

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npj Computational Materials 2022年第1期8卷 1560-1571页

作者： Shikha Saini Joakim Halldin Stenlid Frank Abild-Pedersen suncat center for interface science and catalysis Department of Chemical EngineeringStanford University443 Via OrtegaStanfordCA94305USA suncat center for interface science and catalysis SLAC National Accelerator Laboratory2575 Sand Hill RoadMenlo ParkCA94025USA

The chemisorption energy is an integral aspect of surface chemistry,central to numerous fields such as catalysis,corrosion,and nanotechnology.Electronic-structure-based methods such as the Newns-Anderson model are therefore of great importance in guiding the engineering of material surfaces with optimal properties.However,existing methods are inadequate for interpreting complex,multi-metallic systems.Herein,we introduce a physics-based chemisorption model for alloyed transition metal surfaces employing primarily metal d-band properties that accounts for perturbations in both the substrate and adsorbate electronic states upon interaction.Importantly,we show that adsorbate-induced changes in the adsorption site interact with its chemical environment leading to a second-order response in chemisorption energy with the d-filling of the neighboring atoms.We demonstrate the robustness of the model on a wide range of transition metal alloys with O,N,CH,and Li adsorbates yielding a mean absolute error of 0.13 eV versus density functional theory reference chemisorption energies.

关键词： alloys corrosion chemisorption

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Engineering the interface Between Au Nanoparticles and CoO-Ov to Enhance the Catalytic Performance of 5-Hydroxymethylfurfural(HMF)to 2,5-Dimethylfuran(DMF)

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Chemical Research in Chinese Universities 2024年第1期40卷 47-54页

作者： XIANG Shuang GUO Yong LIU Xiaohui WANG Yanqin Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterResearch Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237P.R.China

The interface between Au and support has attracted extensive interest because of its unique catalytic ability for hydrogen activation in catalytic hydrogenation/hydrogenolysis reactions.Herein,we create the Au-CoO-OV interface in the 1.0%Au/Co3O4-Rod-250 catalyst,which could dissociate H2 via the heterolytic way to yield rich hydride species and achieve excellent catalytic performance in the hydrogenolysis of biomass-derived 5-hydroxymethylfurfural(HMF)to 2,5-dimethylfuran(DMF).The XRD and HRTEM analyses show that Au nanoparticles are uniformly dispersed on CoO-OV surface and in situ DRIFTS spectra show the enhancement of heterolytic dissociation of hydrogen(signals of Au-D and O-D vibration)compared with bare CoO(Co3O4-Rod-250).This work provides insights for fabricating highly active Au-support catalysts for catalytic hydrogenation/hydrogenolysis reactions.

关键词： Au-CoO-OV interface Hydride species Heterolytic dissociation 5-Hydroxymethylfurfural(HMF) 2 5-Dimethylfuran(DMF)

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Keto-form directed hierarchical chiral self-assembly of Schiff base derivatives with amplified circularly polarized luminescence

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Chinese Chemical Letters 2024年第1期35卷 366-370页

作者： Yimeng Sun Yuqian Jiang Jian Jiang Tiesheng Li Minghua Liu Green catalysis center and College of ChemistryZhengzhou UniversityZhengzhou 450001China Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China National Laboratory for Molecular science(BNLMS) CAS Laboratory of ColloidInterface and Chemical ThermodynamicsInstitute of ChemistryChinese Academy of ScienceBeijing 100190China University of Chinese Academy of sciences Beijing 100190China

While enol-keto tautomerism has attracted great interest in Schiff bases and related compounds in solution and crystal states,the self-assembly of energy-unfavored keto form were scarcely investigated.Here,we report a keto-form directed self-assembly of a naphthalene-attached enantiomeric N-salicylideneanil analog L/DGG-Nap accompanied with a significantly amplified circularly polarized luminescence(CPL).It was found that LGG-Nap exists as a mixture of enol and keto form in monomer at a diluted toluene solution.The increment of the concentrations leads to the formation of predominated keto form,which subsequently triggers the self-assembly.Cryo-transmission electron microscopy(Cryo-TEM)revealed that a hierarchical assembly process happened upon increasing the concentration of LGG-Nap in toluene.Individual nanofibers formed at 1×10-4 mol/L and transferred into helical nanofiber bundles in 5×10-3 mol/L.Interestingly,while these is nearly no circular dichroism(CD)or CPL in the monomeric solution,the assembly showed strong CD and CPL.Remarkably,the dissymmetry factor(glum)was significantly amplified from zero in solution through the 0.005 in individual nanofiber to 0.1 in nanofiber bundles.This work demonstrates that the enol-keto tautomerism can be broken and trigger the self-assembly upon increasing the concentration,which can subsequently direct the chiral self-assembly and significantly amplify the dissymmetry factor of assembled CPL materials.

关键词： Enol-keto tautomerism Chiral self-assembly Schiff base Circularly polarized luminescence Nanofiber bundle

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Thiol Ligand-Modified Au for Highly Efficient Electroreduction of Nitrate to Ammonia

Precision Chemistry

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Precision Chemistry 2024年第3期2卷 112-119页

作者： Yuheng Wu Xiangdong Kong Yechao Su Jiankang Zhao Yiling Ma Tongzheng Ji Di Wu Junyang Meng Yan Liu Zhigang Geng Jie Zeng Hefei National Research center for Physical sciences at the Microscale Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of SciencesKey Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education InstitutesDepartment of Chemical PhysicsUniversity of Science and Technology of ChinaHefeiAnhui 230026P.R.China School of Chemistry&Chemical Engineering Anhui University of TechnologyMa’anshanAnhui 243002P.R.China

Electroreduction of nitrate(NO_(3)-)to ammonia(NH_(3))is an environmentally friendly route for NH_(3)production,serving as an appealing alternative to the Haber-Bosch process.Recently,various noble metal-based electrocatalysts have been reported for electroreduction of NO_(3)-.However,the application of pure metal electrocatalysts is still limited by unsatisfactory performance,owing to the weak adsorption of nitrogen-containing intermediates on the surface of pure metal electrocatalysts.In this work,we report thiol ligand-modified Au nanoparticles as the effective electrocatalysts toward electroreduction of NO_(3)-.Specifically,three mercaptobenzoic acid(MBA)isomers,thiosalicylic acid(ortho-MBA),3-mercaptobenzoic acid(meta-MBA),and 4-mercaptobenzoic acid(para-MBA),were employed to modify the surface of the Au nanocatalyst.During the NO_(3)-electroreduction,para-MBA modified Au(denoted as para-Au/C)displayed the highest catalytic activity among these Au-based catalysts.At-1.0 V versus reversible hydrogen electrode(vs RHE),para-Au/C exhibited a partial current density for NH_(3)of 472.2 mA cm^(-2),which was 1.7 times that of the pristine Au catalyst.Meanwhile,the Faradaic efficiency(FE)for NH_(3)reached 98.7%at-1.0 V vs RHE for para-Au/C.The modification of para-MBA significantly improved the intrinsic activity of the Au/C catalyst,thus accelerating the kinetics of NO_(3)-reduction and giving rise to a high NH_(3)yield rate of para-Au/C.

关键词： Ammonia synthesis NO_(3)-electroreduction Au nanoparticles thiol ligand modification electronic structure

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Atomically Dispersed Pt and NiO Clusters Synergistically Enhanced C–O Bond Hydrogenolysis

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CCS Chemistry 2024年第3期6卷 709-718页

作者： Junjuan Yang Sen Luan Minghua Dong Yuxuan Wu Xueqing Xing Xingwu Liu Junfeng Xiang Zhijuan Zhao Shaopeng Li Bin Zhang Huizhen Liu Buxing Han Beijing National Laboratory for Molecular sciences CAS Key Laboratory of Colloid and Interface and ThermodynamicsInstitute of ChemistryChinese Academy of SciencesBeijing 100190 School of Chemical sciences University of Chinese Academy of SciencesBeijing 100049 Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsBeijing 100049 National Energy center for Coal to Liquids Synfuels China Co.Ltd.Huairou DistrictBeijing 101400 center for Physicochemical Analysis and Measurement Institute of ChemistryChinese Academy of SciencesBeijing 100190 Physical science Laboratory Huairou National Comprehensive Science CenterUniversity of Chinese Academy of SciencesBeijing 100049

C–Obond activation is a highly efficient,fundamental strategy in the depolymerization and hydrodeoxygenation of chemicals with oxygen-containing functional groups such as oil,coal,and biomass.Developing efficient catalysts for C–Oactivation with ultralow-loading noble and non-noble metals is highly desirable for the improvement of metal atomic utilization.Herein,bimetallic catalysts with atomically dispersed Pt and NiO clusters on different supports were fabricated,and the prepared Pt^(δ+)-NiO/Nb_(2)O_(5)and Pt^(δ+)-NiO/TiO_(2)showed outstanding activity for the hydrogenolysis of benzyl phenyl ether with>99%yield of phenol and toluene due to the excellent cooperation of atomically dispersed Pt and NiO clusters.The synergy mechanism between Pt and Ni and their respective roles in the bimetallic catalyst for C–O hydrogenolysis were clearly clarified.These findings deepen our understanding of the synergy of the two active components and are expected to provide new design concepts for the development of multicomponents catalysts.

关键词： bimetallic catalysis synergistic effect C-O bond activation hydrogenolysis hydrogen spillover

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Carbon flowers as electrocatalysts for the reduction of oxygen to hydrogen peroxide

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Nano Research 2023年第9期16卷 11556-11563页

作者： Huaxin Gong Lingze Wei Shucheng Chen Zhihua Chen Thomas F.Jaramillo Zhenan Bao Department of Chemical Engineering Stanford UniversityStanfordCA 94305USA suncat center for interface science and catalysis SLAC National Accelerator LaboratoryMenlo ParkCA 94025USA

Small-scale and decentralized production of H_(2)O_(2)via electrochemical reduction of oxygen is of great benefit,especially for sanitization,air and water purification,as well as for a variety of chemical processes.The development of low-cost and highperformance catalysts for this reaction remains a key challenge.Carbon-based materials have drawn substantial research efforts in recent years due to their advantageous properties,such as high chemical stability and high tunability in active sites and morphology.Deeper understanding of structure–activity relationships can guide the design of improved catalysts.We hypothesize that mass transport to active sites is of great importance,and herein we use carbon materials with unique flower-like superstructures to achieve high activity and selectivity for O2 reduction to H_(2)O_(2).The abundance of nitrogen active sites controlled by pyrolysis temperature resulted in high catalytic activity and selectivity for oxygen reduction reaction(ORR).The flower superstructure showed higher performance than the spherical nanoparticles due to greater accessibility to the active sites.Chemical activation improves the catalysts’performances further,driving the production of H_(2)O_(2)to a record-setting rate of 816 mmol·gcat^(−1)·h^(−1)using a bulk electrolysis setup.This work demonstrates the development of a highly active catalyst for the sustainable production of H_(2)O_(2)through rational design and synthetic control.The understanding from this work provides further insight into the design of future carbon-based electrocatalysts.

关键词： carbon materials H_(2)O_(2) oxygen reduction reaction nanostructures

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Revealing the specific role of sulfide and nano-alumina in composite solid-state electrolytes for performance-reinforced ether-nitrile copolymers

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Journal of Energy Chemistry 2024年第4期91卷 628-636页

作者： Haoyang Yuan Changhao Tian Mengyuan Song Wenjun Lin Tao Huang Aishui Yu Department of Chemistry Collaborative Innovation Center of Chemistry for Energy MaterialsShanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsInstitute of New EnergyFudan UniversityShanghai 200438China Laboratory of Advanced Materials Fudan UniversityShanghai 200438China

Composite solid-state electrolytes represent a critical pathway that balances the interface compatibility and lithium-ion conductivity in all-solid-state batteries.The quest for stable and highly ion-conductive combinations between polymers and fillers is vital,but blind attempts are often made due to a lack of understanding of the mechanisms involved in the interaction between polymers and fillers.Herein,we employ in-situ polymerization to prepare a polymer based on an ether-nitrile copolymer with high cathode stability as the foundation and discuss the performance enhancement mechanisms of argyrodite and nano-alumina.With 1%content of sulfide interacting with the polymer at the two-phase interface,the local enhancement of lithium-ion migration capability can be achieved,avoiding the reduction in capacity due to the low ion conductivity of the passivation layer during cycling.The capacity retention after 50cycles at 0.5 C increases from 83.5%to 94.4%.Nano-alumina,through anchoring the anions and interface inhibition functions,eventually poses an initial discharge capacity of 136.8 m A h g^(-1)at 0.5 C and extends the cycling time to 1000 h without short-circuiting in lithium metal batteries.Through the combined action of dual fillers on the composite solid-state electrolyte,promising insights are provided for future material design.

关键词： Composite solid-state electrolytes Lithium metal anode Dual fillers Interfacial ionic conduction Inert nano-alumina

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