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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

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Introducing sulfur to nickel-iron selenide for high-efficiency alkaline seawater electrolysis

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Science China chemistry 2024年第8期67卷 2747-2754页

作者： Xuanwa Chen Yanhui Yu Xingqi Han Huan Wang Yingjie Hua Daoxiong Wu Peilin Deng Juanxiu Xiao Xinlong Tian Jing Li School of Marine Science and Engineering Hainan Provincial Key Lab of Fine ChemistrySchool of Chemistry and Chemical EngineeringHainan UniversityHaikou 570228China Key Laboratory of Advanced Energy Materials chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China Key Laboratory of Electrochemical Energy Storage and Energy Conversion of Hainan Province School of Chemistry and Chemical EngineeringHainan Normal UniversityHaikou 571158China

Seawater electrolysis is an effective way to obtain hydrogen(H_(2))in a sustainable ***,the lack of electrocatalysts with high activity,stability,and selectivity for oxygen evolution reaction(OER)severely hinders the development of seawater electrolysis ***,sulfur-doped nickel-iron selenide nanosheets(S-NiFeSe_(2))were prepared by an ion-exchange strategy and served as highly active OER electrocatalyst for alkaline seawater *** overpotential is 367 m V,and it can run stably for over 50 h at 100 m A cm^(-2).Excitingly,the S-NiFeSe_(2)||Pt/C pair exhibits cell voltage of 1.54 V at 10 m A cm^(-2)under alkaline seawater conditions,which can run smoothly for 100 h without decay,and the efficiency of electricity-tohydrogen(ETH)energy conversion reaches more than 80%.Such electrode,with abundant accessible reactive sites and good corrosion resistance,is a good candidate for seawater ***,density functional theory calculations reveal that the surface sulfur atoms can activate the adjacent Ni sites and decrease the free energy changes of the associated intermediates at the adjacent Ni sites for OER,and the step of~*OH→~*O is the potential rate-limiting *** this work,the true reactive site in nickel-iron selenides is the Ni sites,but not the Fe sites as commonly believed.

关键词： S-doping nickel-iron selenide electrocatalysts oxygen evolution reaction alkaline seawater electrolysis

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Efficient wide-bandgap perovskite solar cells with open-circuit voltage deficit below 0.4 V via hole-selective interface engineering

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Science China chemistry 2024年第6期67卷 2102-2110页

作者： Xiaoyu Ji Shuo Zhang Furong Yu Huidong Zhang Liqing Zhan Yue Hu Wei-Hong Zhu Yongzhen Wu Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision chemistry and Molecular Engineering Shanghai Key Laboratory of Functional Materials ChemistryFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai200237China School of chemistry University of EdinburghKing’s BuildingsEdinburghEH93FJUK

Wide-bandgap mixed-halide perovskite solar cells(WBG-PSCs)are promising top cells for efficient tandem photovoltaics to achieve high power conversion efficiency(PCE)at low ***,the open-circuit voltage(V_(OC))of WBG-PSCs is still unsatisfactory as the V_(OC)-deficit is generally larger than 0.45 ***,we report a buried interface engineering strategy that substantially improves the V_(OC)of WBG-PSCs by inserting amphiphilic molecular hole-selective materials featuring with a cyanovinyl phosphonic acid(CPA)anchoring group between the perovskite and *** assembly and redistribution of CPA-based amphiphilic molecules at the perovskite-substrate buried interface not only promotes the growth of a low-defect crystalline perovskite thin film,but also suppresses the photo-induced halide phase *** energy level alignment between wide-bandgap perovskite and the hole-selective layer is further improved by modulating the substituents on the triphenylamine donor moiety(methoxyls for MPA-CPA,methyls for Me PA-CPA,and bare TPA-CPA).Using a 1.68 e V bandgap perovskite,the Me PA-CPA-based devices achieved an unprecedentedly high V_(OC)of 1.29 V and PCE of 22.3%under standard AM 1.5 *** V_(OC)-deficit(<0.40 V)is the lowest value reported for *** work not only provides an effective approach to decreasing the V_(OC)-deficit of WBG-PSCs,but also confirms the importance of energy level alignment at the charge-selective layers in PSCs.

关键词： cyanovinyl phosphonic acid energy level alignment hole-selective material open-circuit voltage wide-bandgap perovskite

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Mass transfer in heap leaching of weathered crust elution deposited rare earth ore with Al_(2)(SO_(4))_(3) solution

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Journal of Rare Earths 2024年第6期42卷 1175-1181,I0007页

作者： Jingqun Yin Dedong Zeng Jun Tian Yaqing Weng Institute of Applied chemistry Jiangxi Academy of SciencesNanchang330096China School of chemistry and Chemical Engineering Nanchang UniversityNanchang330031China

In order to increase efficiency and avoid NH^(4+)-N pollution in the leaching process of weathered crust elution-deposited rare earth ores,the mass transfer in heap leaching with Al_(2)(SO_(4))_(3) solution was simulated with column elution and experimentally *** results indicate that the leaching yield is also up to 99%for leaching with aluminum sulfate instead of ammonium *** optimal flow rate is 60 mL/h,the height equivalent to a theoretical plate(HETP)is 1.29 mm *** peak value position of RE^(3+)is 60 mL/h,Fe^(3+)is 100 mL/h,however,Al^(3+)is 150 mL/h,and the heap leaching process has kinetic separation effect.

关键词： Raree arths Mass transfer Process optimization Heapleaching Weathered crust elution-deposited rare earth ore

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Upgrading waste NO_(x) into amino acids via electrocatalysis on Co nanoparticles encapsulated in hollow carbon nanofibers

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Science China chemistry 2024年第6期67卷 1946-1952页

作者： Jiahui Xian Kaixing Cai Peisen Liao Shihan Wang Guangqin Li Key Laboratory of Bioinorganic and Synthetic chemistry of Ministry of Education LIFMIGCMESchool of ChemistrySun Yat-Sen UniversityGuangzhou510275China

Electrocatalytic conversion of waste nitrogen oxide(NO_(x))into value-added nitrogenous chemicals,especially amino acid,is an emerging strategy to alleviate NO_(x)***,this process suffers from the coexistence of multiple competitive reactions leading to complex product distribution and low efficiency,and thus the rational design and modulation of efficient catalysts remains a formidable ***,well-designed Co nanoparticles encapsulated in hollow carbon nanofiber(CoHCNF)were constructed to promote the amino acid electrosynthesis via dealing waste NO_(x)coupling with biomass-derived keto *** to the rapid reactant diffusion,electron transport and efficient contact with abundant accessible Co catalytic sites stemmed from the unique hollow nanotubular structure,Co-HCNF manifested impressive glycine synthesis performance in one-pot adopting NO as the nitrogen source with Faradaic efficiency(FE)of 41.7%and a corresponding yield rate of 222.3μmol h^(-1)as well as 120 h robust ***,it also demonstrates an excellent performance with the FE of 42.8%for NO_(3)~-solution as the nitrogen ***,this strategy displays a broad universality for the synthesis of other amino *** work not only highlights the importance of hollow-structuring electrocatalyst towards upgrading wasted NO_(x)species into amino acids,but also promotes the further development of electrosynthetic systems for high-valued N-containing organic chemicals.

关键词： electrocatalysis NO_(x)reduction amino acid porous materials hollow structure

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Catalytically generated noncovalent ammonium dienolate:a versatile platform for the development of organocatalytic asymmetric cascade reactions

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Science China chemistry 2024年第8期67卷 2524-2546页

作者： Jun-Bing Lin Dong-Sheng Ji Peng-Fei Xu State Key Laboratory of Applied Organic chemistry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China Shaanxi Key Laboratory of Chemical Reaction Engineering College of Chemistry and Chemical EngineeringYan’an UniversityYan’an 716000China

Organocatalytic cascade reactions represent a powerful strategy for the rapid construction of complex chiral molecules with multiple stereocenters from simple substrates under mild conditions. The intriguing structural feature and diverse reactivity of catalytically generated dienolate species render them competent and versatile intermediates for the development of practical and valuable cascade reactions. Over the past years, a plethora of innovative and pioneering noncovalent ammonium dienolatemediated cascade reactions have been designed and implemented under the catalysis of chiral organocatalysts, making dienolate activation a general, robust, and complementary method for the functionalization of unsaturated carbonyl compounds and related substances. This review illustrates the recent advances in organocatalytic noncovalent ammonium dienolate-mediated cascade reactions(mainly from 2010 to 2023), including the cascade transformations of ammonium dienolates directly generated from unsaturated ketone/aldehyde, ester/lactone/azlactone, amide/lactam/pyrazolone/oxindole, and alkylidene nitrile compounds. The contents are arranged based on the reaction types of the ammonium dienolates, with an emphasis on cascade 2,5-, 3,5-, and 4,5-difunctionalizations of these intermediates. Furthermore, other cascade reactions involving the 1,3-, 2,3-, and even more complex 3,4,5-reactivities of ammonium dienolates were also discussed. The reaction pathway, reaction stereoinduction, and synthetic applications of the ammonium dienolate-mediated cascade reactions were highlighted throughout the article. As a stimulating and ever-growing research area, the organocatalytic noncovalent ammonium dienolate-mediated cascade reactions are expected to continue demonstrating their magic power for constructing chiral targets in the future and further expanding the boundaries of asymmetric catalysis.

关键词： organocatalysis asymmetric catalysis ammonium dienolate cascade reaction difunctionalization

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Linear paired electrolysis of furfural to furoic acid at both anode and cathode in a multiple redox mediated system

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Green Energy & Environment 2024年第1期9卷 104-113页

作者： Xinxin Li Linchuan Cong Haibo Lin Fangbing Liu Xiangxue Fu Hai-Chao Xu Nan Lin State Key Laboratory of Inorganic Synthesis and Preparative chemistry Jilin UniversityChangchun 130012JilinChina State Key Laboratory of Physical chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina

Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the ***,we report a multiple redox-mediated linear paired electrolysis system,combining the hydrogen peroxide mediated cathode process with the I2 mediated anode process,and realize the conversion of furfural to furoic acid in both side of the dividedﬂow cell *** reasonably controlling the cathode potential,the undesired water splitting reaction and furfural reduction side reactions are *** the galvanostatic electrolysis,the two-mediated electrode processes have good compatibility,which reduce the energy consumption by about 22%while improving the electronic efﬁciency by about 125%.This system provides a green electrochemical synthesis route with commercial prospects.

关键词： Multiple redox mediated system Linear paired electrolysis Furfural Furoic acid

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Increase of chiral sensing ability in host-guest chemistry by magnetic anisotropy

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Science China chemistry 2024年第8期67卷 2775-2782页

作者： Jia-Liang Chen Bin Li Feng Yang Tiesheng Shi Xun-Cheng Su State Key Laboratory of Elemento-organic chemistry Tianjin Key Laboratory of Biosensing and Molecular RecognitionCollege of ChemistryNankai UniversityTianjin 300071China College of chemistry Chemical Engineering and Materials ScienceZaozhuang UniversityZaozhuang 277160China

Enantiomeric molecules generally play distinct functions in chemistry,biology,and *** physical and chemical properties of chiral analytes lay difficulty in discrimination and quantification of the *** report herein an efficient approach of increasing the chiral sensing ability ofβ-cyclodextrin(β-CD),a widely used host molecule,in the hostguest chemistry by magnetic anisotropy.A rigid and chiral lanthanide binding tag was attached to theβ-CD to amplify the changes of nuclear magnetic resonance(NMR)signals in the host-guest recognition *** installation of the paramagnetic lanthanide ion inβ-CD greatly enhances the enantiomeric discrimination up to 30-fold in comparison with the diamagneticβ-CD *** addition,the magnitude of the paramagnetic effects is tunable according to the diverse range of paramagnetic strength of the lanthanide *** reported method significantly increases the chiral sensing ability ofβ-CD,which can be applied to other host *** transferred paramagnetic effects,pseudocontact shifts(PCSs)and paramagnetic relaxation enhancements(PREs),from the host to the guest molecules,are valuable structural restraints to determine the absolute stereochemistry of the chiral *** strategy does not need modification of the analytes and is complementary to the reported analytical methods that rely on the functionalization of the chiral analytes.

关键词： chiral recognition nuclear magnetic resonance host-guest chemistry magnetic anisotropy lanthanide ions

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Covalent triazine frameworks modified by ultrafine Pt nanoparticles for efficient photocatalytic hydrogen production

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Nano Research 2024年第6期17卷 4908-4915页

作者： Xu Han Xueying Ge Wen-Wen He Wangwang Shen Tao Zhou Jian-Sen Wang Rong-Lin Zhong Abdullah MAl-Enizi Ayman Nafady Shengqian Ma School of chemistry and Life Science Advanced Institute of Materials ScienceChangchun University of TechnologyChangchun 130012China Laboratory of Theoretical and Computational chemistry Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China Department of chemistry University of North Texas1508 W.Mulberry St.DentonTX 76201USA Department of chemistry College of ScienceKing Saud UniversityRiyadh 11451Saudi Arabia

Pt nanoparticles(PtNPs)as active species have always been considered as one of the best semiconductor materials for photocatalytic hydrogen *** this study,a Schottky heterojunction has been successfully constructed by evenly loading ultrafine PtNPs onto a triazine-based covalent organic frameworks(COFs).This strategy maintained the high activity of these ultra-small PtNPs while maximizing the utilization of the Pt active *** fabricated PtNPs@covalent triazine-based framework-1(CTF-1)composite accomplished a significantly high rate of hydrogen evolution(20.0 mmol·g^(−1)·h^(−1),apparent quantum efficiency(AQE)=7.6%,atλ=450 nm)with 0.40 wt.%Pt loading,giving rise to a 44-fold-increase in the efficiency of the photocatalytic hydrogen production compared to the pristine *** calculations revealed that the strong electron transfer(Q(Pt)=−0.726 qe,in the analysis of Bader charge,Q(Pt)is the charge quantity transferred from Pt cluster to CTF-1,and qe is the unit of charge transfer quantity)between PtNPs and CTF-1 triggers a strong interaction,which makes PtNPs being firmly attached to the structure of CTF-1,thereby enabling high stability and excellent hydrogen production ***,the hydrogen binding free energy(ΔGH*)of PtNPs@CTF-1 is much lower than that of the unmodified CTF-1,leading to a much lower intermediate state and hence a significant improvement in photocatalytic *** overall findings of this work provide a new platform to incorporate metallic NPs into COFs for the design and fabrication of highly efficient photocatalysts.

关键词： Pt nanoparticles covalent triazine-based framework-1(CTF-1) photocatalysts hydrogen evolution reaction

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Application of "Three-in-One" Strategy Based on MOF-199 in Determination of Phenylenediamine Isomers and Cr(Ⅵ)

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Journal of Analysis and Testing 2024年第1期8卷 28-39页

作者： Yueci Xiang Jiantao Wei Huipeng Sun Ruiyi Zhao Zehua Han Shuangtong Wu Xiaoyan Liu Haixia Zhang State Key Laboratory of Applied Organic chemistry and College of chemistry and Chemical Engineering Lanzhou UniversityLanzhou 730000China

Industry progressing caused the pollutants into the surface and groundwater,including organic pollutants such as phenylenediamine(PD)and heavy metals such as Cr(Ⅵ).Herein,a simple"three-in-one"strategy based on MOF-199 was *** MOF-199 catalytic system could be used for the rapid detection of Cr(Ⅵ)and o-phenylenediamine(OPD)in linear ranges of 0.5-50.0μmol/L and 7.0-250.0μmol/L,with the limits of detection of 0.1 and 0.5μmol/L,*** method can also efficiently discriminate PD isomers in just 15 ***,Cr(Ⅵ)was reduced to Cr(Ⅲ)and the elimination of OPD was carried *** simple synthesis,high sensitivity,easy operation,and low cost,this method presented a potential platform for on-site detection of pollutants in water samples.

关键词： On-site detection “Three-in-one”strategy Phenylenediamine isomers

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