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Journal of Zhejiang University-Science A(Applied Physics & engineering) 2024年第8期25卷 680-686页

作者： Shujie GAO Yongjin HU Zhichang JIANG Xiaoxiang WANG Dong YE Changxing HU College of Quality&Safety engineering China Jiliang UniversityHangzhou 310018China Key Laboratory of Biomass chemical engineering of Ministry of Education Institute of Industrial Ecology and EnvironmentCollege of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China school of Mechatronics and Energy engineering Ningbo Tech UniversityNingbo 315100China

In this study,a series of CuCl_(2)-modified MnO_(x)-CeO_(x)nanorods were synthesized for the oxidation of Hg^(0).The addition of CuCl_(2)resulted in an enhancement in the catalyst’s Hg^(0)oxidation ability,and Hg^(0)oxidation efficiency reached>97%from 150 to 250°*** the MnO_(x)-CeO_(x)catalysts,Mn^(4+)played the role of the active species for Hg^(0)oxidization,but in the CuCl_(2)-doped catalysts Cl−also contributed to Hg^(0)oxidation,conferring the superior performance of these *** introduction of SO_(2) led to a decrease in the availability of Mn^(4+),and the Hg^(0)oxidation efficiency of MnO_(x)-CeO_(x)decreased from about 100%to about 78%.By contrast,CuCl_(2)-promoted samples maintained a Hg^(0)oxidation efficiency of about 100%during the SO_(2) deactivation cycle due to the high reactivity of Cl−.

关键词： Hg^(0)oxidation CuCl_(2)modification MnO_(x)-CeO_(x)nanorods Sulfur resistance O_(x)idation activity

d-d Orbital coupling induced by crystal-phase engineering assists acetonitrile electroreduction to ethylamine

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Journal of Energy Chemistry 2024年第2期89卷 216-225,I0006页

作者： Honggang Huang Yao Chen Hui Fu Cun Chen Hanjun Li Zhe Zhang Feili Lai Shuxing Bai Nan Zhang Tianxi Liu Key Laboratory of Synthetic and biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi 214122JiangsuChina Department of Chemistry KU LeuvenCelestijnenlaan 200FLeuven 3001Belgium College of Chemistry and chemical engineering Qingdao UniversityQingdao 266071ShandongChina

The d-d orbital coupling induced by crystal-phase engineering can effectively adjust the electronic structure of electrocatalysts,thus showing significant catalytic performance,while it has been rarely explored in electrochemical acetonitrile reduction reaction(ARR)to ***,we successfully realize the structural transformation of Pd Cu metallic aerogels(MAs)from face-centered cubic(FCC)to body-centered cubic(BCC)through annealing ***,the BCC Pd Cu MAs exhibit excellent ARR performance with high ethylamine selectivity of 90.91%,Faradaic efficiency of 88.60%,yield rate of 316.0 mmol h^(-1)g^(-1)_(Pd+Cu)and long-term stability for consecutive electrolysis within 20 h at-0.55 V *** hydrogen electrode,outperforming than those of FCC Pd Cu *** the membrane electrode assembly system,BCC Pd Cu MAs also demonstrate excellent ethylamine yield rate of 389.5 mmol h^(-1)g^(-1)_(Pd+Cu).Density functional theory calculation reveals that the d-d orbital coupling in BCC Pd Cu MAs results in an evident correlation effect for the interaction of Pd and Cu sites,which boosts up the Cu sites electronic activities to enhance ARR *** work opens a new route to develop efficient ARR electrocatalysts from the perspective of crystalline structure transformation.

关键词： d-d Orbital coupling Crystal-phase engineering Metallic aerogels Acetonitrile electroreduction reaction Ethylamine

Large-scale chiral spherulites with controllable circularly polarized luminescence in liquid crystal block copolymers film

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Aggregate 2024年第1期5卷 427-435页

作者： Jianan Yuan Xuemin Lu Qinghua Lu school of Chemistry and chemical engineering Shanghai Jiao Tong UniversityShanghaiChina school of chemical Science and engineering Tongji UniversityShanghaiChina

Macroscopic chiral spherulites prepared by hierarchical self-assembly have attracted considerable attention due to their excellent property as chiroptical ***,preparing controllable chiral spherulites in bulk film remains a challenge due to the absent knowledge of the evolution mechanism from the molecule to macroscopic crystal during chiral *** this contribution,chiral macroscopic spherulites were constructed with controllable circularly polarized luminescence(CPL)using enantiomeric tartaric acid and rhodamine B co-assembled with liquid crystal block copolymers,poly(ethylene oxide)-b-poly(methyl methacrylate)bearing azobenzene group side *** was found that the chiral liquid crystal field induced by exogenous chiral molecules was closely related to the formation of macroscopic chiral ***,the transformation of azobenzene cis-trans isomerization under photo-thermal endows films with adjustable *** facile strategy provides a platform to design large-scale chiral structures for chiroptical switching,encryption,and memory storage materials.

关键词： block copolymer circularly polarized luminescence macroscopic chirality self-assembly

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

Efficient ammonia production over e_(g)-occupancy-optimized perovskite electrocatalysts

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Nano Research 2024年第6期17卷 4682-4686页

作者： Mingfa Chen Yu Zhang Fulong Liu Zhenbao Zhang Yuming Dong Yongfa Zhu Heqing Jiang Jiawei Zhu Key Laboratory of Synthetic and biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi 214122China Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266101China school of Chemistry and chemical engineering Linyi UniversityLinyi 276005China Department of Chemistry Tsinghua UniversityBeijing 100084China

Renewable-energy-driven nitrate(NO_(3)^(−))electroreduction to ammonia(NH_(3))(NERA)has been an attractive technology for decarbonizing NH_(3)production and wastewater *** NERA efficiency requires electrocatalysts that are earth-abundant and show fantastic *** we report a semiempirical activity descriptor of eg occupancy(of surface B-site cations)for identifying inexpensive perovskite oxides with extremely high efficacy toward *** establish the descriptor by systematic investigations of more than 10 perovskite *** investigations demonstrate that their intrinsic NERA activities display a volcano-shaped dependence on eg occupancy and the optimized intrinsic activities are accessible at near-1 eg *** could plausibly be attributed to the favorable overlaps between surface adsorbates and vertically-oriented eg *** importantly,utilizing this descriptor,we predict a highly active,selective,and durable NERA electrocatalyst with a composition of Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3−δ)(BSCF).Because of its close-to-1 e_(g)occupancy(i.e.~1.2),the BSCF features a superior NH_(3)production rate of 0.12 g·h^(−1)·mg_(cat.)^(−1)(Faradaic efficiency of 97.8%)that is at top of the volcano plot,and substantially outperforms most NERA electrocatalysts reported in literature.

关键词： perovskite oxide nitrate electroreduction ammonia electrosynthesis eg occupancy

Programmed DNA walkers for biosensors

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Chinese chemical Letters 2024年第9期35卷 119-129页

作者： Chang Liu Tao Wu Lijiao Deng Xuzi Li Xin Fu Shuzhen Liao Wenjie Ma Guoqiang Zou Hai Yang school of Chemistry and chemical engineering Hunan Institute of EngineeringXiangtan 411104China College of Chemistry and chemical engineering Central South UniversityChangsha 410083China

Nowadays,due to excellent biological and polymeric characteristics,DNA has been widely noted as an emerging building block to construct diverse materials for biosensing,in vivo imaging,drug delivery,and disease ***,relying on programmability,predictability,and stability of DNA,DNA walkers have opened new and exciting opportunities in modern life sciences for target detection and biological analysis,which are constructed by self-assembly of DNA or combining DNA with other nanomaterials(e.g.,quantum dots,gold nanoparticles,magnetic nanoparticles,polymers).Compared with conventional nanomaterials(lanthanide-doped upconversion nanoparticles,magnetic nanomaterials,carbon dots,silicon dots,and so on),DNA walkers showed convenient modification,lower biotoxicity,excellent biocompatibility and high biostability,improving the biological ***,with high-speed operating efficiency and sustainable operation,DNA walkers powered by strand displacement reaction or protein enzyme/DNAzyme reaction,have highly sensitive detection and signal amplification abilities,which are applied in biosensing,material assembly and synthesis,and early cancer ***,DNA walkers could be regarded as signal amplifiers,which enhanced the signal transduction and amplified biosensor sensing ***,we systematically and comprehensively summarized the operating principles of various DNA walkers,categorized rational design of the DNA walker,and outlined the application of DNA walker in ***,the challenges and future trends of DNA walkers were discussed.

关键词： DNA walker Biosensors Signal amplification strategies Operating principles Design strategies

Synthesis of 3,5-Diaryl-1,2,4-oxadiazole by One-Pot Homocoupling Reaction

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有机化学 2024年第7期44卷 2251-2256页

作者： Liu Mengjin Xiao Yan Zhou Kai Li Zicheng Huang Wencai school of chemical engineering Sichuan UniversityChengdu 610065

3,5-Diaryl-1,2,4-oxadiazoles were synthesized by homocoupling of chloroarylaldoxime from arylaldoxime and N-chlorosuccinimide(NCS)in the presence of Cs2CO3 in one *** method is suitable for thiophene-3-carbaldehyde,ison-icotinaldehyde and arylaldehyde without active substituent with a yield from 19%to 78%.However,it was not suitable for aliphatic aldehydes,other heteroaromatic aldehydes and benzaldehydes carrying active groups(hydroxyl,amino and carbox-ylic acid).Compared to reported methods,this method uses only aromatic aldoxime as a single *** process is sim-ple,convenient,and green,making it a reliable way to synthesize 3,5-(homo-substituted)-1,2,4-oxadiazoles.

关键词： 1,2,4-oxadiazole homocoupling reaction aldehydes chlorobenzaldoxime cyclic addition

Universal synthesis of metallophthalocyanine covalent organic frameworks as ultra-sensitive multifaceted electrochemical sensor

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Science China Chemistry 2024年第6期67卷 2092-2101页

作者： Qi Liu Qiqi Sun Yuming Zhang Hao Li Wenmiao Chen Yuexing Zhang Sirong Yu Yanli Chen Jianzhuang Jiang school of Materials Science and engineering China University of Petroleum(East China)Qingdao266580China Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials School of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing100083China College of Chemistry and chemical engineering Dezhou UniversityDezhou253023China

The universal synthesis of highly stable covalent organic frameworks(COFs)for ultra-sensitive and multi-component electrochemical detection in different scenarios remains a great ***,a series of metallophthalocyanine-based twodimensional(2D)dioxin(DXI)-linked metalophthalocyanine(MPc)-n DXI-COFs(M=Ni,Zn;n=1,2)are afforded in high yield(80%-96%)by a facile trace-quinoline assisted one-pot condensation of tetracarbonitrile *** X-ray diffraction and electron microscopy investigations disclose their lamellar texture 2D network with AA stacking *** and calculation results elucidate that the 2DXI-linked MPc-2DXI-COFs provide the stronger built-in electronic field and more electrostatic/hydrogen bonding adsorption sites than DXI-linked MPc-DXI-COFs,and the lower electrode reaction Gibbs free energy and stronger adsorption of analytes at Ni Pc than Zn Pc unit,which grants Ni Pc-2DXI-COF excellent sensing properties for various analytes including neurotransmitters,organic pollutants,and heavy metal ions,with high sensitivity and low detection limit of 0.53 to 25.66 *** in binary and ternary systems and even in real-world conditions,simultaneous multi-component detection could be achieved.

关键词： covalent organic framework metallophthalocyanine 2D materials electrochemical sensors multi-component detection

Safety for all temperature zinc-ion batteries

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Journal of Energy Chemistry 2024年第7期94卷 299-301页

作者： Sailin Liu Zaiping Guo school of chemical engineering the University of AdelaideSA 5000Australia

Zinc-ion batteries(ZIBs)have emerged as a promising candidate in the grid scale energy storage,offering an alternative to conventional lithium-ion ***,as research and development efforts in this field progress,it becomes increasingly important to address potential hazards associated with flammable gases and electrolyte *** future paper aims to raise awareness of safety issues that may be overlooked and underscore two primary temperature-induced hazards:long-term cycling H_(2) gas accu-mulation and flammable organic *** evaluate various electrolytes aimed at minimizing gas pro-duction and improving high-temperature ***,we emphasize the effectiveness of electrolyte modifications,especially co-solvent approach in addressing the above safety concerns and suggest pathways for formulating practical safe ***,apart from examining the inherent electrochemical stability window(EsW)of the electrolyte,we urge consideration of side reaction prod-ucts on electrode interfaces and high temperatures as factors influencing a battery's EsW.

关键词： battery electrolyte offering