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Journal of Environmental Sciences 2024年第3期137卷 395-406页

作者： Fangzhi Duan Yongfeng Zhu Yan Liu Aiqin Wang Key Laboratory of Clay Mineral Applied Research of Gansu Province Center of Eco-material and Green ChemistryLanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China center of materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China

Porous materials applied in environmental remediation have received researchers'extensive attention recently,but the related green and convenient preparation method is rarely ***,we recommended a green and convenient strategy for the fabrication of porous material via aqueous foam templates,which was synergistically stabilized by Codonopsis pilosula(CP)and clay minerals of attapulgite(APT).The characterization results revealed that the APT was modified by organic molecules leached from CP and anchored at the air-water interface,which improved the foam stability *** novel porous material of polyacrylamide/Codonopsis pilosula/attapulgite(PAM/CP/APT)templated from the aqueous foam via a polymerization reaction had excellent adsorption capacity for the cationic dyes methyl violet(MV)and methylene blue(MB),and the adsorption capacity can reach 755.85 mg/g and557.64 mg/g,*** importantly,the adsorption capacity of spent adsorbent material was still over 200 mg/g after being recycled five times through a simple carbonization process,and then it was added to the plant pot,the total biomass was increased by about86.42%.This study provided a green and sustainable pathway for the preparation,application and subsequent processing of porous materials.

关键词： Porous material Aqueous foam Atapulgite Adsorption Cationic dyes Sustainable utilization

p-d Orbital Hybridization Engineered Single-Atom Catalyst for Electrocatalytic Ammonia Synthesis

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Energy & Environmental materials 2024年第2期7卷 123-129页

作者： Jingkun Yu Xue Yong Siyu Lu green Catalysis center and College of Chemistry Zhengzhou University Department of chemistry University of Sheffield

The rational design of metal single-atom catalysts（SACs） for electrochemical nitrogen reduction reaction（NRR） is challenging. Two-dimensional metal–organic frameworks（2DMOFs） is a unique class of promising SACs. Up to now, the roles of individual metals, coordination atoms, and their synergy effect on the electroanalytic performance remain unclear. Therefore, in this work, a series of 2DMOFs with different metals and coordinating atoms are systematically investigated as electrocatalysts for ammonia synthesis using density functional theory calculations. For a specific metal, a proper metalintermediate atoms p-d orbital hybridization interaction strength is found to be a key indicator for their NRR catalytic activities. The hybridization interaction strength can be quantitatively described with the p-/d-band center energy difference（Δd-p）, which is found to be a sufficient descriptor for both the p-d hybridization strength and the NRR performance. The maximum free energy change（ΔGmax） and Δd-p have a volcanic relationship with OsC4（Se）4located at the apex of the volcanic curve, showing the best NRR performance. The asymmetrical coordination environment could regulate the band structure subtly in terms of band overlap and *** work may shed new light on the application of orbital engineering in electrocatalytic NRR activity and especially promotes the rational design for SACs.

关键词： first-principle calculations Nitrogen reduction p-d orbital hybridization single-atom catalysts

A meso–molecular muscle based on copillar[5]arenes

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Chinese Chemical Letters 2024年第3期35卷 308-311页

作者： Yu Yao Peiling Zhang Dan Zhou Zhinan Lai Shijun Li Feihe Huang Zibin Zhang College of material Chemistry and Chemical EngineeringKey Laboratory of Organosilicon Chemistry and Material TechnologyMinistry of EducationKey Laboratory of Organosilicon Material TechnologyHangzhou Normal UniversityHangzhou 311121China Department of chemistry Stoddart Institute of Molecular ScienceZhejiang UniversityHangzhou 310027China green Catalysis center and College of chemistry Zhengzhou UniversityZhengzhou 450001China

A meso–molecular muscle was prepared by capping the[c2]daisy chain based on a mono-functionalized copillar[5]arene with an imidazolium group in its *** its crystal structure,we observed that it was a cyclic dimer composed of two mirror image subcomponents,a pR-and a pS-copillar[5]*** conformations were fixed by the doubly interlocked mechanical *** comparison of the^1H NMR and COSY spectra,we found that the length of this meso–molecular muscle could be controlled not only by the solvents,but also by the counter anions.

关键词： Pillararenes Molecular muscles [c2]daisy chains Planar chirality

Synergism of solar-driven interfacial evaporation and photo-Fenton Cr(Ⅵ) reduction by sustainable Bi-MOF-based evaporator from waste polyester

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Journal of Energy chemistry 2024年第7期94卷 527-540页

作者： Zifen Fan Jie Liu Huajian Liu Lijie Liu Yan She Xueying Wen Huiyue Wang Guixin Hu Ran Niu Jiang Gong Key Laboratory of material chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureHubei Engineering Research Center for Biomaterials and Medical Protective MaterialsSemiconductor Chemistry CenterSchool of Chemistry and Chemical EngineeringHuazhong University of Science andTechnologyWuhan430074HubeiChina

The integration of interfacial solar steam generation and photocatalytic degradation technology has pro-vided a promising platform to simultaneously produce freshwater and degrade ***,con-structing low-cost,multi-functional evaporators for treating Cr(Ⅵ)-polluted water remains challenging,and the synergistic mechanism on Cr(Ⅵ)reduction is ***,we propose the combined strategy of ball milling and solution mixing for the sustainable production of Bi-MOF microrod from waste poly(ethylene terephthalate),and construct Bi-MOF-based solar evaporators for simultaneous photo-Fenton Cr(Ⅵ)reduction and freshwater ***,the evaporator comprised of Bi-MOF microrod and graphene nanosheet possesses high light absorption,efficient photothermal conversion,and good hydro-philic *** to the advantages,the hybrid evaporator exhibits the evaporation rate of 2.16 kg m^(-2) h^(-1) and evaporation efficiency of 87.5%under 1 kW m^(-2) of *** integrating with photo-Fenton reaction,the Cr(Ⅵ)reduction efficiency is 91.3%,along with the reaction kinetics of 0.0548 min^(-1),surpassing many advanced *** the outdoor freshwater production and Cr(Ⅵ)reduction,the daily accumulative water yield is 5.17 kg m^(-2) h^(-1),and the Cr(Ⅵ)reduction efficiency is 99.9%.Furthermore,we prove that the localization effect derived from the interfacial solar-driven evap-oration enhances H_(2)O_(2) activation for the photo-Fenton reduction of Cr(Ⅵ).Based on the result of density functional theory,Bi-MOF microrod provides rich active centers for H_(2)O_(2) activation to produce active sites such as e-or-O_(2).This study not only proposes a new strategy to construct multi-functional solar evaporators for freshwater production and catalytic reduction of pollutants,but also advances the chem-ical upcycling of waste polyesters.

关键词： Interfacial solar steam generation Cr(VI)reduction Photo-Fenton reaction Metal-organic framework Waste plastic upcycling

Highly selective and eco-friendly dihydroisoquinoline synthesis via Cu/Co synergistic catalysis in Cu NPs@MOFs catalyst under mild conditions

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Science China chemistry 2024年第5期67卷 1561-1568页

作者： Peng-Fei Guo Ze-Long Liang Yue-E Jiao Hang Xu Bin Zhao Key Laboratory of Advanced Energy material chemistry Renewable Energy Conversion and Storage CenterDepartment of ChemistryNankai UniversityTianjin 300071China

3,4-Dihydroisoquinoline(DHIQ)is an important precursor used in the production of drugs for treating cancer,HIV,Alzheimer's disease,*** studies on DHIQ synthesis show low catalytic selectivity due to the susceptible over-oxidation feedstock of1,2,3,4-tetrahydroisoquinoline(THIQ),which often requires alkali ***,it is desirable yet challenging to explore a highly selective and efficient oxydehydrogenation capacity for DHIQ synthesis under eco-friendly reaction ***,a novel framework 1 was synthesized,exhibiting 1D channels with the size of 4.6 A×9.6 A and high solvent/p H/thermal stability.A stable framework allows it to encapsulate Cu nanoparticles(NPs)to form Cu NPs@1-x(x=1,2,3,and 4)with varying loading amounts of Cu NPs at 2.0 wt%,3.0 wt%,4.0 wt%,and 6.0 wt%,*** NPs@1-3 could selectively catalyze the reaction from THIQ to DHIQ with a high selectivity of 98%and a recorded turnover frequency(TOF)of 22.1 h-1under eco-friendly mild *** corresponding catalytic activity can maintain at least five recyclings and can be further applied to gram-scale ***,the efficient preparation of DHIQ catalyzed by Cu NPs@1-3 could be realized even under air ***,the anticancer molecule precursor synthesis of 6,7-dimethoxy-3,4-dihydroisoquinoline was also selectively catalyzed by Cu NPs@*** investigations revealed that high catalytic performance can be attributed to the stable framework and the synergistic catalytic effect of the loaded Cu NPs and Co metal *** importantly,this work represents the first example of MOF catalysts for selectively thermo-catalytic DHIQ synthesis and demonstrates a simple approach to obtain efficient catalysts for selective oxydehydrogenation in the production of unsaturated compounds.

关键词： metal-organic frameworks Cu NPs@MOFs 3 4-dihydroisoquinoline selective oxydehydrogenation synergistic catalysis

Acidic electroreduction CO_(2)to formic acid via interfacial modification of Bi nanoparticles at industrial-level current

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Nano Research 2024年第7期17卷 5817-5825页

作者： Tian Dong Hongdong Li Zhenhui Wang Yanling Geng Rui Chang Xiaofeng Tian Jianping Lai Shouhua Feng Lei Wang Key Laboratory of eco-Chemical Engineering International Science and Technology Cooperation Base of Eco-Chemical Engineering and Green ManufacturingCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China Shandong Engineering Research center for Marine Environment Corrosion and Safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042China

Electrocatalytic CO_(2)reduction reaction(CO_(2)RR)in acidic media is a promising approach to overcome the unavoidable formation of carbonates in alkaline or neutral ***,the proton-rich environment near the catalyst surface favors hydrogen evolution reactions(HER),leading to lower energy efficiency of the desired products,especially in industrial-level current ***,quaternary ammonium cationic surfactant(cetyltrimethylammonium bromide(CTAB))was introduced into acidic electrolyte to modulate the interfacial microenvironment,which greatly enhanced CO_(2)electroreduction to formic acid(HCOOH)at the Bi/C nanoparticles *** a Bi/C nanoparticles electrode with CTAB added,constant production of formic acid was enabled with a cathodic energy efficiency of>40%and maximum FE_(HCOOH)(FE=Faradaic efficiency)of 86.2%at−400 mA·cm^(−2)over 24 *** with in-situ attenuated total reflection Fourier transform infrared spectroscopy,the concentration of*OCHO intermediates significantly increased after CTAB modification,confirming that the hydrophobic interface microenvironment formed by dynamic adsorption of positively charged long alkyl chains on Bi/C nanoparticle electrodes inhibited HER and improved the selectivity of CO_(2)RR to HCOOH.

关键词： acidic media CO_(2)electrolysis electrolyte additive hydrophobic interfacial microenvironment industrial-level current

Regulate electric double layer for one-step synthesize and modulate the morphology of(oxy)hydroxides

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Nano Research 2024年第5期17卷 3675-3683页

作者： Jiaxin Liu Yue Shi Yanli Gu Zheng Lv Liang Zhao Yu Yang Tianrong Zhan Jianping Lai Lei Wang State Key Laboratory Base of eco-Chemical Engineering International Science and Technology Cooperation Base of Eco-chemical Engineering and Green ManufacturingCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China Shandong Engineering Research center for Marine Environment Corrosion and Safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042China

FeOOH have received considerable attention due to their natural abundance and *** the significant progress achieved,the one-step synthesis of integrated FeOOH is still a major ***,the current research on FeOOH catalyst still suffers from the unclear mechanism of controlling ***,density functional theory(DFT)calculations and X-ray photoelectron spectroscopy(XPS)demonstrated the strong electron-capturing and hydrogen absorption ability of Co in FeOOH,which further promotes the formation and stabilization of *** used a one-step electrodeposition method to synthesize Co introduced FeOOH integrated electrocatalyst and propose to introduce ions with different valence states to regulate the morphology of FeOOH by precise modulation of electric double layer(EDL)composition and *** prepared Co-FeOOH-K^(+)has a larger electrochemically active surface area(ECSA)(325 cm^(2))and turnover frequency(TOF)value(0.75 s^(-1)).In the electrochemical experiments of an alkaline anion exchange membrane electrolyzer,Co-FeOOH-K^(+)shows better oxygen evolution performance than commercial RuO_(2) under industrial production conditions and has good industrial application prospects.

关键词： integrated(oxy)hydroxides electrodeposition electric double layer(EDL) oxygen evolution reaction(OER) morphology regulation

In situ Hydrothermal Oxidation of Ternary FecoNi Alloy Electrode for Overall Water Splitting

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Energy & Environmental materials 2024年第2期7卷 165-174页

作者： Yuwei Chen Lixia Yang Chao Li Yuqiu Wu Xiao Lν Hairen Wang Jun'e Qu Key Laboratory for the green Preparation and Application of Functional materials Hubei Key Laboratory of Polymer Materials School of Materials Science and Engineering Hubei University Faculty of material science and chemistry China University of Geosciences

Exploring noble metal-free catalyst materials for high efficient electrochemical water splitting to produce hydrogen is strongly desired for renewable energy *** this article,a novel bifunctional catalytic electrode of insitu-grown type for alkaline water splitting based on FecoNi alloy substrate has been successfully prepared via a facile one-step hydrothermal oxidation route in an alkaline hydrogen peroxide *** shows that the matrix alloy with the atom ratio 4:3:3 of Fe:Co:Ni can obtain the best catalytic performance when hydrothermally treated at 180℃ for18 h in the solution containing 1.8 M hydrogen peroxide and 3.6 M sodium *** as-prepared Fe0.4Co0.3Ni0.3-1.8 electrode exhibits small overpotentials of only 184 and 175 mV at electrolysis current density of10 mA cm-2for alkaline OER and HER processes,*** overall water splitting at electrolysis current density of 10 mA cm-2can be stably delivered at a low cell voltage of 1.62 *** characteristics including the large specific surface area,the high surface nickel content,the abundant catalyst species,the balanced distribution between bivalent and trivalent metal ions,and the strong binding of in-situ naturally growed catalytic layer to matrix are responsible for the prominent catalytic performance of the Fe0.4Co0.3Ni0.3-1.8 electrode,which can act as a possible replacement for expensive noble metal-based materials.

关键词： alkaline water electrolysis bifunctional electrocatalyst FecoNi alloy hydrothermal oxidation in-situ growing

Boosting thermal stability and crystallization of closed-loop-recyclable biodegradable poly(p-dioxanone) by end-group regulation

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Science China chemistry 2024年第2期67卷 642-651页

作者： Jin Lei Zhu-Xin Gui Wan-Ting Xiong Gang Wu Si-Chong Chen Yu-Zhong Wang The Collaborative Innovation center for eco-Friendly and Fire-Safety Polymeric materials(MoE) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)State Key Laboratory of Polymer Materials EngineeringCollege of ChemistrySichuan UniversityChengdu610064China

A chemically closed-loop-recyclable biodegradable polymer,poly(p-dioxanone)(PPDO),is one of the ideal candidates for single-use plastic products due to its suitability for different application ***,when PPDO wastes can be collected,its monomer p-dioxanone(PDO) will be obtained through chemical recycling of these wastes;when cannot be collected,the wastes are able to be biodegraded into harmless ***,unsatisfied thermal stability and low crystallization rate of PPDO restrict its wider ***,based on end-group regulation,we simultaneously realized the significant enhancement of thermal stability and crystallization of PPDO through the simple melt processing with tributyl phosphite(TBP) or triphenyl phosphite(TPP).The model reactions were conducted to investigate the reaction mechanism and theoretical products during the preparation of PPDO/phosphite *** kinds of phosphites were proved to act as the end-capped reagent and chain extender in the melt processing,while TBP presented better *** a result,the activation energy of thermal decomposition was largely elevated,and the unprecedented T_(5%)(the temperature at a weight loss of 5%) and Tmax(the temperature at a maximum rate of weight loss) of PPDO were obtained,i.e.,T_(5%)of ~330 ℃ and Tmaxof ~385 ℃ in N_(2) atmosphere,T_(5%)of ~240 ℃ and Tmaxof ~317 ℃ in air atmosphere,***,the increased crystallization rate,crystallinity,crystalline orderliness,and realizable monomer recovery(yield >90%,purity >99.9%) of PPDO/phosphite compounds were confirmed.

关键词： poly(p-dioxanone) phosphite thermal stability crystallization end-group regulation

Multi-stimuli-responsive aggregation-induced emission copper iodide cluster

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Science China chemistry 2024年第4期67卷 1193-1197页

作者： Bo Li Yuan-Yuan Liu Peng Luo Ye-Ru Liu Ying-Jun Chen Kai Li Shuang-Quan Zang College of chemistry and Pharmacy Engineering Nanyang Normal UniversityNanyang 473061China green Catalysis center and College of chemistry Zhengzhou UniversityZhengzhou 450001China

Stimuli-responsive luminescent materials have attracted significant attention in the development of smart photoactive materials for both fundamental research and technological *** this work,a new copper iodide cluster(1)with aggregationinduced emission(AIE)characteristic,was obtained combining Cu_(4)I_(4) core with rhodamine B derivative ligand.1 has reversible and distinct multi-stimuli-responsive luminescence for external temperature,volatile organic compound,and mechanical ***,1 exhibited unusual large blue shift(84 nm)after being ground,which originated from the change of intermolecular ***,1 exhibits high oxygen quenching efficiency for 82.2% at 1 *** studies showed that the multi-stimuli-responsive luminescence properties of 1 can be attributed to the regulation of cluster-centered luminescence process,metal-to-ligand charge transfer process,halide-to-metal charge transfer luminescence process and aggregationinduced barrier to oxygen *** work not only reports an AIE copper iodide cluster,but also provides a new strategy to develop multi-stimuli-responsive luminescence materials.

关键词： copper iodide cluster aggregation-induced emission multi-stimuli-response