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Upper-rim-modified thioether thiacalix[4]arene used for liquid-liquid extraction of Au(Ⅲ)and Pd(Ⅱ)in hydrochloric acid medium

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Chinese Journal of Chemical Engineering 2024年第2期66卷 110-118页

作者： Sheng Wan Rong Xie Jianhong Fan Kewen Tang Department of chemistry and Chemical Engineering Hunan Institute of Science and TechnologyYueyang 414006China

Gold(Au)and palladium(Pd)play an increasing role in the production and human life;Therefore,it is of great significance to study their recovery.A 5,11,17,23-tetra-ethylthio-25,26,27,28-tetra-hydroxyl thiacalix[4]arene(TCAET)was synthesized specifically for the capture of Au(Ⅲ)and Pd(Ⅱ)from HCl medium by liquid-liquid *** a 0.1 mol·L^(-1)HCl medium,the transfer of Au(Ⅲ)and Pd(Ⅱ)from the aqueous phase to the organic phase was highly efficient,with a transfer ratio of 100%for Au(Ⅲ)and 98%for Pd(Ⅱ).Furthermore,the extraction equilibrium time for Au(Ⅲ)was just 5 ***'s method data demonstrated that TCAET formed complexes with Au(Ⅲ)and Pd(Ⅱ)in a ratio of 2:3 and 1:1,respectively,during the extraction *** showed high selectivity toward Pd(Ⅱ)and Au(Ⅲ)over other competing metal ***,both Au(Ⅲ)and Pd(Ⅱ)could be successfully stripped from the loaded organic phases with a 1.0 mol·L^(-1)thiourea in 0.5 mol·L^(-1)HCl and 0.5 mol·L^(-1)thiourea in 0.5 mol·L^(-1)HCl,*** obtained from five consecutive extraction-stripping cycles showed good reusability of TCAET toward Au(Ⅲ)and Pd(Ⅱ)*** conclusion can provide a certain reference for thiacalixarene in the recovery of precious metal species.

关键词： Thiacalixarene Upper-rim modification Liquid-liquid extraction Precious metal Thioether

Regio-and Stereoselective Polymerization of Bio-based Ocimene by Rare-Earth Metal Catalysts

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Chinese Journal of Polymer Science 2024年第2期42卷 223-229,I0008页

作者： Qi-Yuan Wang Li-Peng Sang Zhen Zhang Yang Jiang Hui Tian Xia Zhao Xiang Guo Shi-Hui Li State Key Laboratory of Polymer Physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei230026China Science and Technology on Aerospace Chemical Power Laboratory Hubei Institute of Aerospace ChemotechonologyXiangyang441003China Shanxi Coal Chemical Industry Technology Research institute Xi’an710000China Hubei institute of Aerospace Chemotechonology Xiangyang441003China

Coordination polymerization of renewable β-ocimene has been investigated using asymmetric diiminophosphinate lutetium complex1, β-diketiminate yttrium complex 2, bis(phosphino)carbazolide yttrium complex 3, half-sandwich benzyl fluorenyl scandium complex 4 and pyridyl-methylene-fluorenyl rare-metal complexes 5a–5c. Complexes 1, 4 and 5a–5c show trans-1,2-regioselectivities and high activities, of which 5c exhibits excellent isoselectivity(mmmm>99%). Conversely, complexes 2 and 3 promote β-ocimene polymerization to produce isotactic cis-1,4-polyocimenes(cis-1,4>99%, mm>95%). Diblock copolymers cis-1,4-PIP-block-cis-1,4-POc and cis-1,4-PBD-block-cis-1,4-POc are obtained in one-pot reactions of β-ocimene with isoprene and butadiene using complex 3. Epoxidation and hydroxylation of polyocimene afford functionalized polyolefins with enhanced T_(g)(from-20 ℃ to 79 ℃ and 74 ℃) and hydrophilicity.

关键词： Biobased monomer Terpenes Ocimene Rare-earths Polymerization Regio/stereoselectivity Elastomer

Pd-catalyzed intermolecular Si–O formation via Si–C activation

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Science China chemistry 2024年第8期67卷 2661-2669页

作者： Shuang Liu Yu-Shu Chen Yichen Wu Peng Wang State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesShanghai 200032China School of chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China College of Material chemistry and Chemical Engineering Key Laboratory of Organosilicon Chemistryand Material Technology of Ministry of EducationHangzhou Normal UniversityHangzhou 311121China

The development of efficient Si–O bond formation reaction with 100% atom-economy, excellent functional group tolerance, and broad scope under mild conditions is highly desired due to the prevalence of silanol, silyl ether, and their derivatives in synthetic chemistry and materials science. Here, we have realized the Pd-catalyzed Si–O formation reaction via a Si–C activation approach with 100% atom-economy by employing silacyclobutanes(SCBs) and various hydroxy-containing substrates, including water,alcohols, phenols, and silanols. This protocol features a broad substrate scope, remarkable functional compatibility and mild conditions, providing a series of silanols, silyl ethers in high efficiency. Notably, this protocol could also be used for selective protection of hydroxy functionalities, and for the access of a class of novel polymers containing Si–O main chain. Preliminary mechanistic studies unveiled that this reaction underwent a Pd-catalyzed concerted ring-opening mechanism.

关键词： Si–O formation Si–C activation palladium silacyclobutane silanol silyl ether

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Bio-Based Rigid Polyurethane Foams for Cryogenic Insulation

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Journal of Renewable Materials 2024年第3期12卷 585-602页

作者： Laima Vevere Beatrise Sture Vladimir Yakushin Mikelis Kirpluks Ugis Cabulis Latvian State institute of Wood chemistry RigaLV-1006Latvia

Cryogenic insulation material rigid polyurethane(PU)foams were developed using bio-based and recycled *** obtained from tall oil fatty acids produced as a side stream of wood biomass pulping and recycled polyethylene terephthalate were used to develop rigid PU foam *** 4th generation physical blowing agents with low global warming potential and low ozone depletion potential were used to develop rigid PU foam cryogenic insulation with excellent mechanical and thermal *** rigid PU foams had a thermal conductivity coefficient as low as 0.0171 W/m·K and an apparent density of 37-40 kg/m^(3).The developed rigid PU foams had anisotropic compression strength properties,which were higher parallel to the foaming ***,the compression strength was also influenced by the type of applied bio-based *** bio-based polyols with higher OH group functionality delivered higher crosslinking density of polymer matrix;thus,the mechanical properties were also *** mechanical strength of the foams increased when materials were tested at liquid nitrogen temperature due to the stiffening of the polymer *** thermal properties of the developed materials were determined using differential scanning calorimetry,dynamic mechanical analysis,and thermogravimetric analysis ***,the developed rigid PU foams had good adhesion to the aluminium substrate before and after applying cyroshock and an excellent safety coefficient of *** PU foams developed using Solstice LBA delivered adhesion strength of~0.5 MPa and may be considered for application as cryogenic insulation in the aerospace industry.

关键词： Cryogenic insulation polyurethanes tall oil 4th generation physical blowing agents

Vacancy engineering induced reaction kinetics enhancement of cobalt metaphosphate for pH-universal hydrogen evolution

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Nano Research 2024年第5期17卷 3879-3887页

作者： Yuting Chen Tian Meng Zhicai Xing Yueying Yan Yang Yang Bohan Yao Dewen Wang Xiurong Yang State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China

Developing efficient pH-universal hydrogen evolution reaction(HER)catalysts is critical in the field of water electrolysis,however,which is severely hampered by the sluggish kinetics in alkaline ***,a ruthenium(Ru)incorporation induced vacancy engineering strategy is firstly proposed to precisely construct oxygen vacancy(V_(O))-riched cobalt-ruthenium metaphosphate(CRPO)for high-efficiency pH-universal *** V_(O) modifies the electronic structure,improves the superficial hydrophilic and gas spillover capacity,it also reduces the coordination number of Ru atoms and regulates the coordination *** calculations indicate that Ru tends to adsorb H_(2)O and H^(*),whereas V_(O) tends to adsorb OH^(-),which greatly promotes the H_(2)O adsorption and the dissociation of HO-H ***,CRPO-2 exhibits remarkable HER performance,the mass activity is about 18.34,21.73,and 38.07 times higher than that of Pt/C in acidic,neutral,and alkaline media,respectively,at the same time maintain excellent *** findings may pave a new avenue for the rational design of electrocatalysts toward pH-universal water electrolysis.

关键词： cobalt metaphosphate pH-universal hydrogen evolution reaction(HER) vacancy engineering low-coordination atoms oxygen vacancy

Preparation and Characterization of Biobased Dehydroabietyl Polyethylene Glycol Glycidyl Ether-Grafted Hydroxyethyl Cellulose with High Emulsifying Property

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Journal of Renewable Materials 2024年第1期12卷 103-117页

作者： Zhengqing Ding Quan Yang Xinyan Yan Feng Gu Xujuan Huang Zhaosheng Cai School of Chemical and chemistry Yancheng Institute of TechnologyYancheng224051China

Dehydroabietyl polyethylene glycol glycidyl ether-grafted hydroxyethyl cellulose(HEC)polymer surfactant(DA(EO)5GE-g-HEC)was prepared using ring-opening polymerization with biobased rosin and hydroxyethyl cellulose as *** polyethylene glycol glycidyl ether(DA(EO)5GE)was formed by condensation of dehydroabietyl alcohol polyoxyethylene ether(Rosin derivative:DA(EO)5H)and *** grafting degree of DA(EO)5GE-g-HEC was manipulated by adjusting the mass ratio of HEC and DA(EO)5GE and confirmed by *** to the formula,when m(HEC)/m(DA(EO)2GE)was 1:1~1:5,the grafting rate of DA(EO)5GE in DA(EO)5GE-g-HEC varied from 34.43%to 38.33%.The surface activity and foam properties of DA(EO)5GE-g-HEC aqueous solution were *** results showed that with the increase in grafting rate,the critical micellar concentration(CMC)in aqueous solution changed from 1.28 to 0.96 g/*** results of the thermogravimetric analysis showed that the temperature range of the main stage of mass loss of DA(EO)5GE-g-HEC was 310°C~410°C,and the thermal decomposition processes of the samples with five mass ratios were *** oil in water emulsion was prepared by choosing cyclohexane as the oil phase and DA(EO)5GE-g-HEC as the *** effect of DA(EO)5GE-g-HEC mass fraction on emulsion particle size and stability was *** results suggested that when the oil-water ratio was 8:2 with 0.4%emulsifier,the emulsion droplets were the smallest in terms of particle size and were the most *** rheological test results showed that the apparent viscosity decreased with the increase in shear rate and showed a typical elastic gel phenomenon.

关键词： Rosin hydroxyethyl cellulose surfactant emulsion rheological behaviour

Atomically dispersed Fe sites on hierarchically porous carbon nanoplates for oxygen reduction reaction

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Journal of Energy chemistry 2024年第3期90卷 7-15,I0002页

作者： Ruixue Zheng Qinglei Meng Hao Zhang Teng Li Di Yang Li Zhang Xiaolong Jia Changpeng Liu Jianbing Zhu Xiaozheng Duan Meiling Xiao Wei Xing State Key Laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026AnhuiChina Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesJiangsu Key Laboratory of Advanced Negative Carbon TechnologiesSoochow UniversitySuzhou 215123JiangsuChina State Key Laboratory of Polymer Physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina

Developing cost-effective,robust and stable non-precious metal catalysts for oxygen reduction reaction(ORR) is of paramount importance for electrochemical energy conversion devices such as fuel cells and metal-air *** Fe-N-C single atom catalysts(SACs) have been hailed as the most promising candidate due to the optimal binding strength of ORR intermediates on the Fe-N_(4) sites,they suffer from serious mass transport limitations as microporous templates/substrates,i.e.,zeolitic imidazolate frameworks(ZIFs),are usually employed to host the active *** by this challenge,we herein develop a hydrogen-bonded organic framework(HOF)-assisted pyrolysis strategy to construct hierarchical micro/mesoporous carbon nanoplates for the deposition of atomically dispersed Fe-N_(4) *** a design is accomplished by employing HOF nanoplates assembled from 2-aminoterephthalic acid(NH_(2)-BDC) and p-phenylenediamine(PDA) as both soft templates and C,N *** from the structural merits inherited from HOF templates,the optimized catalyst(denoted as Fe-N-C SAC-950) displays outstanding ORR activity with a high half-wave potential of 0.895 V(*** hydrogen electrode(RHE)) and a small overpotential of 356 mV at 10 mA cm^(-2) for the oxygen evolution reaction(OER).More excitingly,its application potential is further verified by delivering superb rechargeability and cycling stability with a nearly unfading charge-discharge gap of 0.72 V after 160 *** dynamics(MD) simulations reveal that micro/mesoporous structure is conducive to the rapid mass transfer of O_(2),thus enhancing the ORR *** situ Raman results further indicate that the conversion of O_(2) to~*O_(2)-the rate-determining step(RDS) for Fe-N-C *** work will provide a versatile strategy to construct single atom catalysts with desirable catalytic properties.

关键词： Fe single atom catalysts Oxygen reduction reaction Mesoporous structure Active sites Zinc-air battery

Recent progress in photocatalytic NAD(P)H regeneration for photocatalytic-enzymatic-coupling system

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Frontiers of Chemical Science and Engineering 2024年第4期18卷 1-24页

作者： Wei Lan Maodi Wang Huicong Dai Qihua Yang Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Zhejiang Key Laboratory for Reactive Chemistry on Solid SurfacesInstitute of Physical ChemistryZhejiang Normal UniversityJinhua 321004China

The enzymatic redox reactions in natural photosynthesis rely much on the participation of cofactors,with reduced nicotinamide adenine dinucleotide/nicotinamide adenine dinucleotide phosphate(NADH/NADPH)or their oxidized form(NAD+/NADP+)as an important redox *** photocatalytic regeneration of expensive and unstable NADH/NADPH in vitro is an important process in enzymatic reduction and has attracted much research *** different types of photocatalysts have been developed for photocatalytic NADH/NADPH regeneration,the efficiency is still relatively *** elucidate the key factors affecting the performance of photocatalytic NADH/NADPH regeneration is helpful to rationally design the photocatalyst and improve the photocatalytic *** this paper,we overview the recent progress in photocatalytic NADH/NADPH regeneration with the focus on the strategies to improve the visible light adsorption,the charge separation and migration efficiency,as well as the surface reaction,which jointly determine the overall photocatalytic regeneration *** potential development of photocatalytic NADH/NADPH regeneration and photocatalyticenzymatic-coupling system is prospected finally.

关键词： photocatalytic-enzymatic coupling NAD(P)H regeneration photocatalysis efficiency

A multi-parameter-induced activation of gas therapeutic platform to remarkably amplify photodynamic therapy efficacy

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Science China chemistry 2024年第7期67卷 2403-2411页

作者： Jie Sun Ziwen Zhang Hongyu Wu Xuemei Dong Chengjun Dong Lixin Sun Zhiqian Guo Yingchao Liu Xianfeng Gu Chunchang Zhao Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center Institute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Department of medicinal chemistry School of PharmacyFudan UniversityShanghai 201203China Shandong Provincial Hospital Affiliated to Shandong First Medical University Shandong First Medical University&Shandong Academy of Medical ScienceJinan 250021China

Gas therapy(GT)combined with photodynamic therapy(PDT)is an effective strategy to compensate for the PDT limitation caused by the hypoxic tumor microenvironment,which can greatly improve PDT *** uncontrolled leakage of gas molecules during delivery seriously hinders its practical biological ***,we report a multifunction nanomedicine that enables precise gas therapy(including carbon monoxide(CO)release and H_(2)S depletion)using a multi-parameter-induced activation gas release strategy,enlarging the PDT *** nanomedicine uses a disulfide bond to covalently link a photosensitizer with the CO donor 3-hydroxyflavone(3-HF).The disulfide bond can be specifically consumed in H_(2)S-rich tumor areas,releasing the CO donor(3-HF),and also depleting H_(2)*** importantly,the photo-controlled production of^(1)O_(2)can induce 3-HF precise release of CO in the tumor *** H_(2)S,light,and^(1)O_(2)multi-parameter-induced activation of gas release strategy ensures the accuracy of GT to amplify PDT *** expected,in vitro and in vivo investigations show that GT makes up for the PDT limitation,exhibiting the highest tumor therapeutic *** multi-parameter-activated design strategy provides a new way to improve the precision and efficacy of multimodal synergistic therapy of tumors.

关键词： gas therapy precision gas release hydrogen sulfide depletion photodynamic therapy multimodal synergistic therapy

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