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Ligand effect in surface atomic sites of group VI B transition metals on ultrathin Pt nanowires for enhanced oxygen reduction

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Nano Research 2024年第6期17卷 5298-5304页

作者： Yuwei He Yueguang Chen Renjie Wu Zhihe Xiao Mengxian Li Chunfeng Shi Leyu Wang state key laboratory of chemical Resource engineering College of ChemistryBeijing University of Chemical TechnologyBeijing 100029China state key laboratory of Petroleum Molecular and Process engineering SINOPEC Research Institute of Petroleum Processing Co.Beijing 100083China

Increasing the utilization efficiency of platinum is critical for advancing proton exchange-membrane fuel cells(PEMFCs).Despite extensive research on catalysts for the cathodic oxygen reduction reaction(ORR),developing highly active and durable Pt-based catalysts that can suppress surface dealloying in corrosive acid conditions remains ***,we report a facile synthesis of bimetallic ultrathin PtM(M=Mo,W,and Cr)nanowires(NWs)composed of group VI B transition metal atomic sites anchored on the *** NWs possess uniform sizes and well-controlled atomic *** to PtW and PtCr catalysts,the PtMo0.05 NWs exhibit the highest half-wave potential of 0.935 V and a mass activity of 1.43 A·mgPt^(−1).Remarkably,they demonstrate a remarkable 23.8-fold enhancement in mass activity compared to commercial Pt/C for ORR,surpassing previously reported Pt-based ***,the PtMo NWs cathode in membrane electrode assembly tests achieves a remarkable peak power density of 1.443 W·cm^(−2)(H_(2)-O_(2)conditions at 80℃),which is 1.09 times that of commercial Pt/*** ligand effect in the bimetallic surface not only facilitates strong coupling between Mo(4d)and Pt(5d)atomic orbitals to hinder atom leaching but also modulates the d-states of active site,significantly optimizing the adsorption of key oxygen(*O and*OH)species and accelerating the rate-determining step in ORR pathways.

关键词： ligand effect oxygen reduction reaction group VI B transition metal ultrathin nanowires multiple oxygen species

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Nickel-catalyzed arylcyanation of alkenes via cyano group translocation:access to 1,n-dinitriles or 4-amino nitriles

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Science China Chemistry 2024年第9期67卷 2975-2981页

作者： Xiaohong Li Shenfan Wang Xiangxiang Fu Donghui Xing Zeyuan Fu Yuanfu Deng Huanfeng Jiang Liangbin Huang state key laboratory of Pulp and Paper engineering School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China

Herein,a nickel-catalyzed arylcyanation of unactivated alkenes via cyano group translocation with aryl boronic acids has been *** transformations provided a robust approach to constructing structurally diverse 1,n-dinitriles or 4-amino nitriles from easily prepared and commercially available starting *** cyano group translocation was achieved,involving the addition into the intramolecular C–N triple bond followed by the retro-Thorpe *** studies revealed that high temperature and CsHCO_(3) as the base were crucial for the cyano group translocation.

关键词： arylcyanation nickel catalysis cyano group translocation 1 n-dinitriles 4-amino nitriles

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Nano-alumina@cellulose-coated separators with the reinforcedconcrete-like structure for high-safety lithium-ion batteries

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Chinese Journal of chemical engineering 2024年第4期68卷 83-93页

作者： Zhihao Yang Li Chen Jian Xue Miaomiao Su Fangdan Zhang Liangxin Ding Suqing Wang Haihui Wang Guangdong Provincial key Lab of Green chemical Product Technology School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China Beijing key laboratory of Membrane Materials and engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

Separators play a critical role in the safety and performance of lithium-ion ***,commercial polyolefin separators are limited by their poor affinity with electrolytes and low melting *** this work,we constructed a reinforced-concrete-like structure by homogeneously dispersing nano-Al_(2)O_(3) and cellulose on the separators to improve their stability and *** this reinforcedconcrete-like structure,the cellulose is a reinforcing mesh,and the nano-Al_(2)O_(3) acts as concrete to support the *** constructing the reinforced-concrete-like structure,the separators exhibit good stability even at 200℃(thermal shrinkage of 0.3%),enhanced tensile strain(tensile stress of 133.4 MPa and tensile strains of 62%),and better electrolyte wettability(a contact angle of 6.5°).Combining these advantages,the cells with nano-Al_(2)O_(3)@cellulose-coated separators exhibit stable cycling performance and good rate ***,the construction of the reinforced-concretelike structure is a promising technology to promote the application of lithium-ion batteries in extreme environments.

关键词： Alumina Nanomaterials Lithium-ion batteries Membranes Cellulose Reinforced-concrete-like structure

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Molecular surface functionalization of In_(2)O_(3) to tune interfacial microenvironment for enhanced catalytic performance of CO_(2) electroreduction

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Nano Research 2024年第3期17卷 1242-1250页

作者： Suwen WangQiang GaoCui Xu Shuai Jiang Mengyang Zhang Xianjun Yin Hui-Qing Peng Bin Liu Yu-Fei Song state key laboratory of chemical Resource engineering Beijing Advanced Innovation Center for Soft Matter Science and EngineeringCollege of ChemistryBeijing University of Chemical TechnologyBeijing 100029China

Indium-based materials(e.g.,In_(2)O_(3))are a class of promising non-noble metal-based catalysts for electroreduction of carbon dioxide(CO_(2)).However,competitive hydrogen reduction reaction(HER)on indium-based catalysts hampers CO_(2) reduction reaction(CO_(2)RR)*** herein tune the interfacial microenvironment of In_(2)O_(3) through chemical graft of alkyl phosphoric acid molecules using a facile solution-processed strategy for the first time,which is distinguished from other researches that tailor intrinsic activity of In_(2)O_(3) *** surface functionalization of alkyl phosphoric acids over In_(2)O_(3) is demonstrated to remarkably boost CO_(2) *** example,octadecylphosphonic acid modified In_(2)O_(3) exhibits Faraday efficiency for H_(2) H_(2) H_(2)(FE)of as low as 6.6%and FEHCOOH of 86.5%at-0.67 V ***,which are far superior to parent In_(2)O_(3) counterparts(FE of 24.0%and FEHCOOH of 63.1%).Moreover,the enhancing effect of alkyl phosphoric acid functionalization is found to be closely related to the length of alkyl *** virtue of comprehensive experimental characterizations and molecular dynamics simulations,it is revealed that the modification of alkyl phosphoric acids significantly alters the interface microenvironment of the electrocatalyst,which changes the electrocatalyst surface from hydrophilic and aerophobic to hydrophobic and *** this case,the water molecules are pushed away and more CO_(2) molecules are trapped,increasing local CO_(2) concentration at In_(2)O_(3) active sites,thus leading to the significantly enhanced CO_(2)RR and suppressed *** work highlights the importance of regulating the interfacial microenvironment of inorganic catalysts by molecular surface functionalization as a means for promoting the electrochemical performance in electrosynthesis and beyond.

关键词： carbon dioxide(CO_(2))electroreduction interfacial microenvironment molecular surface functionalization In_(2)O_(3)catalyst water and CO_(2)diffusion

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Piezoelectric-enhanced n-TiO2/BaTiO3/p-TiO2 heterojunction for highly efficient photoelectrocatalysis

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Green Energy & Environment 2024年第9期9卷 1466-1476页

作者： Minhua Ai Zihang Peng Xidi Li Faryal Idrees Xiangwen Zhang Ji-Jun Zou Lun Pan key laboratory for Green chemical Technology of the Ministry of Education School of Chemical Engineering and Technology Tianjin University Collaborative Innovative Center of chemical Science and engineering (Tianjin) Haihe laboratory of Sustainable chemical Transformations department of Physics University of the Punjab Quaid-e-Azam Campus

Charge separation is critical for achieving efficient solar-to-hydrogen conversion,whereas piezoelectric-enhanced photoelectrochemical（PEC） systems can effectively modulate band bending and charge ***,we design an n-Ti O2/Ba Ti O3/p-Ti O2（TBTm） heterojunction in which the piezoelectric Ba Ti O3layer is sandwiched between n-Ti O2and p-Ti *** built-in electric field of TBTm can provide a strong driving force to accelerate carrier separation and prolong carrier ***,the TBT3 achieves a prominent photocurrent density,as high as 2.13 m A cm-2at 1.23 V versus reversible hydrogen electrode （RHE）,which is 2.4-and 1.5-times higher than Ti O2and Ti O2–Ba Ti O3heterojunction,*** by mechanical deformation,the induced dipole polarization can further regulate built-in electric fields,and the piezoelectric photocurrent density of TBT3-800 is 2.84 times higher than Ti O2at 1.23 V *** due to the construction of *** work provides a piezoelectric polarization strategy for modulating the built-in electric field of heterojunction for PEC system.

关键词： Photoelectrochemical Piezoelectric polarization Heterojunction Charge separation

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Solvent effects on Diels-Alder reaction in ionic liquids:A reaction density functional study

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Chinese Journal of chemical engineering 2024年第2期66卷 180-188页

作者： Zijiang Dou Weiqiang Tang Peng Xie Shuangliang Zhao Guangxi key laboratory of Petrochemical Resource Processing and Process Intensification Technology and School of Chemistry and chemical engineering Guangxi UniversityNanning 530004China state key laboratory of chemical engineering and School of chemical engineering East China University of Science and TechnologyShanghai 200237China

Extensive experimental studies have been performed on the Diels-Alder(DA)reactions in ionic liquids(ILs),which demonstrate that the IL environment can significantly influence the reaction rates and ***,the underlying microscopic mechanism remains *** this work,the multiscale reaction density functional theory is applied to explore the effect of 1-butyl-3-methylimidazolium hexafluorophosphate([BMIM][PF_(6)])solvent on the reaction of cyclopentadiene(CP)with acrolein,methyl acrylate,or *** analyzing the free energy landscape during the reaction,it is found that the polarization effect has a relatively small influence,while the solvation effect makes both the activation free energy and reaction free energy *** addition,the rearrangement of local solvent structure shows that the cation spatial distribution responds more evidently to the reaction than the anion,and this indicates that the cation plays a dominant role in the solvation effect and so as to affect the reaction rates and selectivity of the DA reactions.

关键词： Solvent effect Ionic liquids Diels-Alder reaction Reaction density functional theory

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NIR-Ⅱ responsive Janus nanoparticles amplify immunogenic cell death for enhanced cancer immunotherapy

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Science China(Technological Sciences) 2024年第1期67卷 321-329页

作者： CHEN BeiBei GUO KangLi WANG HaoRan XU Fu-Jian WANG JuLin ZHAO NaNa state key laboratory of chemical Resource engineering Beijing University of Chemical TechnologyBeijing 100029China key laboratory of Biomedical Materials of Natural Macromolecules(Beijing University of chemical Technology) Beijing Laboratory of Biomedical MaterialsBeijing University of Chemical TechnologyBeijing 100029China College of Materials Sciences and engineering Beijing University of Chemical TechnologyBeijing 100029China Beijing key laboratory of Electrochemical Process and Technology for Materials Beijing University of Chemical TechnologyBeijing 100029China

Immunotherapy brings new hope for tumor treatment by inducing immunogenic cell death(ICD)of tumor ***,insufficient immunogenicity and low immune response rate greatly limit antitumor ***,by optimizing the composition and morphology,the rational design of Janus nanoparticles composed of Fe_(3)O_(4) nanospheres and SiO_(2)nanorods was realized for enhanced cancer immunotherapy through amplified *** glucose oxidase(GOx)was loaded by the Janus nanoparticles,the resultant M-FS-GOx consumes glucose at tumor sites to generate gluconic acid and hydrogen peroxide(H_(2)O_(2))for starvation therapy while the H_(2)O_(2)supply promotes the production of highly toxic·OH to achieve effective chemodynamic therapy(CDT).Under a 1064 nm light irradiation,the photothermal effect of M-FS-GOx enhances the enzyme activity of GOx for improved starvation ***,both tumor-associated antigens released during the process of ICD and the intrinsic immunoadjuvant property of M-FS-GOx stimulate dendritic cell maturation to activate antitumor immune *** work provides a promising strategy for the construction of Janus nanoparticles to achieve enhanced cancer immunotherapy through combination therapy-amplified ICD.

关键词： Janus nanoparticles immunogenic cell death cancer immunotherapy

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Highly selective electrosynthesis of 3,4-dihydroisoquinoline accompanied with hydrogen production over three-dimensional hollow CoNi-based microarray electrocatalysts

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Nano Research 2024年第4期17卷 2509-2519页

作者： Yu Xin Liyu Chen Yingwei Li Kui Shen Guangdong Provincial key Lab for Green chemical Product Technology School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China state key laboratory of Pulp and Paper engineering School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China

Electrocatalytic oxidation reaction of biomass-based derivatives is an excellent candidate to replace water oxidation for obtaining both value-added products and hydrogen(H_(2)),but the exploration of competent electrocatalysts is still highly ***,two new types of three-dimensional self-supported hollow microarrays containing CoNi layered double hydroxide(CoNi-LDH)and N-doped carbon nanosheets decorated with CoNi alloyed nanoparticles(CoNi-NC)on carbon cloth(CC)are prepared,which are further used as efficient electrocatalysts for tetrahydroisoquinoline(THIQ)electrooxidation and hydrogen evolution reaction(HER),*** demonstrate that the Co-modulated electronic environment for Ni(II)/Ni(Ⅲ)redox-looping in CoNi-LDH is the main factor to boost the selectivity of 3,4-dihydroisoquinoline(DHIQ)for the indirect electrooxidation process of *** functional theory(DFT)calculations reveal that the Ni(Ⅲ)/Co(Ⅲ)dual sites of CoNi-LDH exhibit enhanced adsorption for THIQ but poorer adsorption for DHIQ compared to pure Co(Ⅲ)or Ni(Ⅲ).Therefore,the Ni(Ⅲ)/Co(Ⅲ)dual sites can effectively inhibit the peroxidation of DHIQ to isoquinoline(IQ)over CoNi-LDH,thus improving the selectivity of DHIQ to nearly 100%,much higher than that of its pure Ni ***,CC@CoNi-NC can deliver high HER activity with low overpotential(40 mV@10 mA·cm^(-2))and high exchange current density(3.08 mA·cm^(-2)).Impressively,the assembled flow-cell device with CC@CoNi-LDH anode and CC@CoNi-NC cathode only requires low cell voltage and electricity consumption of 1.6 V and 3.50 kWh per cubic meter of H_(2)(@25 mA·cm^(-2)).

关键词： highly selective electrosynthesis dihydroisoquinolines hydrogen evolution reaction metal-organic frameworks hollow microarrays

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Enhancing photoresponsiveness of metal-organic polyhedra by modifying microenvironment

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Nano Research 2024年第6期17卷 5712-5717页

作者： Long Zheng Peng Tan Qian Song Sheng-Tao Wang Min Li Xiao-Qin Liu Lin-Bing Sun state key laboratory of Materials-Oriented chemical engineering Jiangsu National Synergetic Innovation Center for Advanced Materials(SICAM)College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China

Photoresponsiveness of materials is critical to their tunability and efficiency in terminal *** metal-organic polyhedra(PMOPs)feature intrinsic pores and remote controllability,but aggregation of PMOPs in solid state hampers their photoresponsiveness ***,we report the construction of a new PMOP(Cu_(24)(C_(16)H_(12)N_(2)O_(4))_(12)(C_(18)H_(22)O_(5))12,denoted as MOP-PR-LA),where long alkyl(LA)chains act as the intermolecular poles,propping against adjacent PMOP molecules to create individual microenvironment benefiting the isomerization of photoresponsive(PR)*** ultraviolet(UV)-and visible-light irradiation,MOP-PR-LA is much easier to isomerize than the counterpart MOP-PR without *** propylene adsorption,MOP-PR has a low change of adsorption capacity(9.9%),while that of MOP-PR-LA reaches 58.6%.Density functional theory calculations revealed that PR in the cis state has a negative effect on adsorption,while the trans state of PR favors *** work might open an avenue for the construction of photoresponsive materials with high responsiveness and controllability.

关键词： photoresponsive adsorption metal-organic polyhedra azobenzene long alkyl chains propylene capture

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Low-energy-consumption temperature swing system for CO_(2) capture by combining passive radiative cooling and solar heating

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Green Energy & Environment 2024年第3期9卷 507-515页

作者： Ying-Xi Dang Peng Tan Bin Hu Chen Gu Xiao-Qin Liu Lin-Bing Sun state key laboratory of Materials-Oriented chemical engineering Jiangsu National Synergetic Innovation Center for Advanced Materials(SICAM)College of Chemical EngineeringNanjing Tech UniversityNanjing211816China

Temperature-swing adsorption(TSA)is an effective technique for CO_(2) capture,but the temperature swing procedure is ***,we report a low-energy-consumption system by combining passive radiative cooling and solar heating for the uptake of CO_(2) on commercial activated carbons(CACs).During adsorption,the adsorbents are coated with a layer of hierarchically porous poly(vinylidene fluoride-co-hexafluoropropene)[P(VdF-HFP)HP],which cools the adsorbents to a low temperature under sunlight through radiative *** desorption,CACs with broad absorption of the solar spectrum are exposed to light irradiation for *** heating and cooling processes are completely driven by solar *** tests under mimicked sunlight using the CACs show that the performance of this system is comparable to that of the traditional ***,under real sunlight irradiation,the adsorption capacity of the CACs can be well maintained after multiple *** present work may inspire the development of new temperature swing procedures with little energy consumption.

关键词： CO_(2)capture Solar heating Passive radiative cooling Temperature swing adsorption

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