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Ionic liquid-assisted preparation of hydroxyapatite and its catalytic performance for decarboxylation of itaconic acid

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Chinese Journal of chemical Engineering 2024年第3期67卷 9-15页

作者： Shutong Pang Hualiang An Xinqiang Zhao Yanji Wang Hebei provincial key laboratory of Green chemical technology and Efficient Energy Saving Tianjin Key Laboratory of Chemical Process SafetySchool of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300130China

The synthesis of methacrylic acid from biomass-derived itaconic acid is a green route,for it can get rid of the dependence on fossil resource.In order to solve the problems on this route such as use of a preciousmetal catalyst and a corrosive homogeneous alkali,we prepared a series of hydroxyapatite catalysts by an ionic liquid-assisted hydrothermal method and evaluated their catalytic performance.The results showed that the ionic liquid[Bmim]BF_(4) can affect the crystal growth of hydroxyapatite,provide fluoride ion for fluorination of hydroxyapatite,and adjust the surface acidity and basicity,morphology,textural properties,crystallinity,and composition of hydroxyapatite.The[Bmim]BF4 dosage and hydrothermal temperature can affect the fluoride ion concentration in the hydrothermal system,thus changing the degree of fluoridation of hydroxyapatite.High fluoride-ion concentration can lead to the formation of CaF_(2) and thus significantly decrease the catalytic performance of hydroxyapatite.The hydrothermal time mainly affects the growth of hydroxyapatite crystals on the c axis,leading to different catalytic performance.The suitable conditions for the preparation of this fluoridized hydroxyapatite are as follows:a mass ratio of[Bmim]BF4 to calcium salt=0.2:1,a hydrothermal time of 12 h,and a hydrothermal temperature of 130℃.A maximal methacrylic acid yield of 54.7%was obtained using the fluoridized hydroxyapatite under relatively mild reaction conditions(250℃ and 2 MPa of N_(2))in the absence of a precious-metal catalyst and a corrosive homogeneous alkali.

关键词： Ionic liquid Hydroxyapatite Itaconic acid Methacrylic Decarboxylation reaction

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Multiresponsive,easy-reversible,and dual-visual Pt(Ⅱ)salt nanostructures for advanced anti-counterfeiting application

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Nano Research 2024年第1期17卷 372-381页

作者： Zhen Su§ Depeng Li§ Lixin Zhang Si Tian Yuhong Su Xiaoyun Hu Duan Xiong Qingqing Guan key laboratory of oil and gas Fine chemicals Ministry of Education College of Chemical EngineeringXinjiang UniversityUrumqi 830017China

Smart materials that integrate multi-stimuli response,full reversibility,and dual-visual read-out channel are highly desired for anticounterfeiting and information encryption applications.Herein,we developed a multiresponsive perchlorate terpyridyl Pt(Ⅱ)nano complex which could undergo fully reversible conversion between three forms stimulated by water or formaldehyde molecule due to the extent of Pt–Pt interaction.Meanwhile,a dual-visual channel,i.e.,the colorimetric channel changed from yellow to orange or red and the corresponding luminescent channel from orange to orange-red or red,has also been found.The weak and equivalent strength of ion-dipole interaction and hydrogen bond that generated between formaldehyde/water and Pt(II)salt result in the easy-control reversibility between the three forms.Furthermore,by introducing different polymer matrices,1Cl·ClO_(4)@PMMA(1Cl·ClO_(4):[Pt(tpy)Cl]·ClO4,tpy:2,2':6',2''-terpyridine),PMMA:poly(methyl methacrylate))and 1Cl·ClO4@PVA(PVA:polyvinyl alcohol)are successfully constructed,which exhibit different reversible behaviors since the PMMA and PVA matrix exert different influences on the strength of hydrogen-bond.Those smart Pt(II)salt nanostructures present great potential for high-security-level anticounterfeiting application.

关键词： Pt(II)complex multiresponse reversibility anticounterfeiting information encryption

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Impact of Annealing on the Melt Recrystallization of a-PDLA/α-PLLA Double-layered Films

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Chinese Journal of Polymer Science 2024年第2期42卷 230-238,I0009页

作者： Yun-Peng Li Hao-Ran Shen Shao-Juan Wang Hao Zhang Jian Hu Rui Xin Xiao-Li Sun Shou-Ke Yan key laboratory of Rubber-Plastics Ministry of Education/Shandong Provincial Key Laboratory of Rubber-plasticsQingdao University of Science&TechnologyQingdao266042China State key laboratory of chemical Resource Engineering Beijing University of Chemical TechnologyBeijing100029China

Poly(lactic acid)(PLA) as a bio-based polymer with biodegradability and biocompatibility has attracted much attention. To manipulate its properties for different applications, regulation of crystal structure and crystalline morphology becomes an attractive research topic. In this work, the structure evolution of layered samples containing an amorphous poly(D-lactide)(PDLA) layer and a crystalline poly(L-lactide)(PLLA)layer with highly oriented edge-on α lamellar crystals after annealing at 150 ℃ or/and after melt-recrystallization has been studied by AFM, FTIR,and TEM combined with electron diffraction. The results demonstrate that melt recrystallization of the as-prepared sample leads to the formation of abundant randomly oriented PLA stereo-complex(PLA SC) crystals. Annealing at 150 ℃ results in the formation of a small amount of oriented PLA SC crystals at the interface. These PLA SC crystals show great impact on the recrystallization behavior of sample after melting at 190 ℃ and then crystallizing at 90 ℃. First, they impede the mutual diffusion of the overlying PDLA and underlying PLLA, and thus reduce their stereocomplexation ability as manifested by the decreased amount of PLA SC crystals. Second, they act as substrate to initiate the epitaxial crystallization of the overlying PDLA and underlying PLLA, which ensures the production of a highly oriented structure of PDLA and PLLA after melt recrystallization again.

关键词： Poly(L-lactide) Poly(D-lactide) Double layer Stereocomplex

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Applications of genetic code expansion technology in eukaryotes

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Protein & Cell 2024年第5期15卷 331-363页

作者： Qiao-ru Guo Yu J.Cao State key laboratory of chemical Oncogenomic Guangdong Provincial Key Laboratory of Chemical GenomicsPeking University Shenzhen Graduate SchoolShenzhen 518055China Institute of chemical Biology Shenzhen Bay LaboratoryShenzhen 518132China

Unnatural amino acids(UAAs)have gained significant attention in protein engineering and drug development owing to their ability to introduce new chemical functionalities to proteins.In eukaryotes,genetic code expansion(GCE)enables the incorporation of UAAs and facilitates posttranscriptional modification(PTM),which is not feasible in prokaryotic systems.GCE is also a powerful tool for cell or animal imaging,the monitoring of protein interactions in target cells,drug development,and switch regulation.Therefore,there is keen interest in utilizing GCE in eukaryotic systems.This review provides an overview of the application of GCE in eukaryotic systems and discusses current challenges that need to be addressed.

关键词： genetic code expansion unnatural amino acid eukaryotes basic research therapeutic applications

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Enhanced stability of nitrogen-doped carbon-supported palladium catalyst for oxidative carbonylation of phenol

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Chinese Journal of chemical Engineering 2024年第1期65卷 19-28页

作者： Xiaojing Liu Ruohan Zhao Hao Zhao Zhimiao Wang Fang Li Wei Xue Yanji Wang Hebei provincial key laboratory of Green chemical technology and High Efficient Energy Saving School of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300130China Tianjin key laboratory of chemical Process Safety Tianjin 300130China Hebei Industrial technology Research Institute of Green chemical Industry Huanghua 061100China

Enhancing the stability of supported noble metal catalysts emerges is a major challenge in both science and industry.Herein,a heterogeneous Pd catalyst(Pd/NCF)was prepared by supporting Pd ultrafine metal nanoparticles(NPs)on nitrogen-doped carbon;synthesized by using F127 as a stabilizer,as well as chitosan as a carbon and nitrogen source.The Pd/NCF catalyst was efficient and recyclable for oxidative carbonylation of phenol to diphenyl carbonate,exhibiting higher stability than Pd/NC prepared without F127 addition.The hydrogen bond between chitosan(CTS)and F127 was enhanced by F127,which anchored the N in the free amino group,increasing the N content of the carbon material and ensuring that the support could provide sufficient N sites for the deposition of Pd NPs.This process helped to improve metal dispersion.The increased metal-support interaction,which limits the leaching and coarsening of Pd NPs,improves the stability of the Pd/NCF catalyst.Furthermore,density functional theory calculations indicated that pyridine N stabilized the Pd^(2+)species,significantly inhibiting the loss of Pd^(2+)in Pd/NCF during the reaction process.This work provides a promising avenue towards enhancing the stability of nitrogen-doped carbon-supported metal catalysts.

关键词： Supported Pd catalyst N-doped carbon Amphiphilic triblock copolymer Pyridinic nitrogen Stability

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Relationship between hydrogenation degree and pyrolysis performance of jet fuel

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Chinese Journal of chemical Engineering 2024年第4期68卷 35-42页

作者： Qing Liu Tinghao Jia Lun Pan Jijun Zou Xiangwen Zhang key laboratory for Green chemical and technology School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Haihe laboratory of Sustainable chemical Transformations Tianjin 300192China Zhejiang Institute of Tianjin University Ningbo 315201China Zhejiang provincial key laboratory of Advanced chemical Engineering Manufacture technology College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China

Understanding the relationship between the chemical composition and pyrolysis performance of endothermic hydrocarbon fuel(EHF)is of great significance for the design and optimization of advanced EHFs.In this work,the effect of deep hydrogenation on the pyrolysis of commercial RP-3 is investigated.Fuels with different hydrogenation degrees were obtained by the partially and completely catalytic hydrogenation and their pyrolysis performances were investigated using an apparatus equipped with an electrically heated tubular reactor.The results show that with the increase of hydrogenation degree,fuel conversion almost remains constant during the pyrolysis process(500e650C,4 MPa);however,the heat sink increases slightly,and the anti-coking performance significantly improves,which are highly related to their H/C ratios.Detailed characterisations reveal that the difference of the pyrolysis performance can be ascribed to the content of aromatics and cycloalkanes:the former are prone to initiate secondary reactions to form coking precursors,while the latter could act as the hydrogen donor and release hydrogen,which will terminate the radical propagation reactions and suppress the coke deposition.This work should provide the guidance for upgrading EHFs by modulating the composition of EHFs.

关键词： RP-3 Fuel Pyrolysis Hydrogenation Deposition

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Apically guiding electron/mass transfer reaction induced by Ag/FeNx Mott-Schottky effect within a hollow star reactor toward high performance zinc-air batteries

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Journal of Energy Chemistry 2024年第8期95卷 106-116页

作者： Kaixiang Shi Kaixin Wang Tong Li Junhao Li Jie Ren Xu Li Yonggang Min Zhouguang Lu Wei Tan Quanbing Liu Guangdong provincial laboratory of Chemistry and Fine chemical Engineering Jieyang Center(Rongjiang laboratory) Guangdong University of Technology Guangzhou key laboratory of Clean Transportation Energy Chemistry Guangdong Provincial Key Laboratory of Plant Resources Biorefinery School of Chemical Engineering and Light Industry Guangdong University of Technology key laboratory of Electrochemical Energy Storage and Energy Conversion of Hainan Province School of Chemistry and Chemical Engineering Hainan Normal University School of Materials and Energy Guangdong University of Technology Department of Materials Science and Engineering Southern University of Science and Technology

The disparity in the transfer of carriers（electrons/mass） during the reaction in zinc-air batteries（ZABs）results in sluggish kinetics of the oxygen reduction reaction（ORR） and oxygen evolution reaction（OER）,along with elevated overpotentials,thereby imposing additional constraints on its utilization.Therefore,the pre-design and target-development of inexpensive,high-performance,and long-term stable bifunctional catalysts are urgently needed.In this work,an apically guiding dual-functional electrocatalyst（Ag-FeNx-N-C） was prepared,in which a hierarchical porous nitrogen-doped carbon with three-dimensional（3D） hollow star-shaped structure is used as a substrate and high-conductivity Ag nanoparticles are coupled with iron nitride（FeNx） nanoparticles.Theoretical calculations indicate that the Mott-Schottky heterojunction as an inherent electric field comes from the two-phase bound of Ag and FeNx,of which electron accumulation in the FeNxphase region and electron depletion in the Ag phase region promote orientated-guiding charge migration.The effective modulation of local electronic structures felicitously reforms the d-band electron-group distribution,and intellectually tunes the masstransfer reaction energy barriers for both ORR/OER.Additionally,the hollow star-s haped hierarchical porous structure provides an apical region for fast mass transfer.Experimental results show that the halfwave potential for ORR is 0.914 V,and the overpotential for OER is only 327 mV at 10 mA cm-2.A rechargeable ZAB with Ag-FeNx-N-C as the air cathode demonstrates long-term cycling performance exceeding 1500 cycles（500 h）,with a power density of 180 mW cm-2.Moreover,when employing AgFeNx-N-C as the air cathode,flexible ZABs demonstrate a notable open-circuit voltage of 1.42 V and achieve a maximum power density of 65.6 mW cm-2.Ag-FeNx-N-C shows guiding electron/mass transfer route and apical reaction microenvironment for the electrocatalyst architecture in the exploration prospects of ZABs.

关键词： Apically guiding effect Bifunctional catalysis Hollow star structure Mott-Schottky effect Zinc-air batteries

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Recycling of waste aluminum scraps to fabricate sulfidated zero-valent iron-aluminum particles for enhanced chromate removal

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Journal of Environmental Sciences 2024年第4期138卷 650-659页

作者： Yahui Zhang Liguo Zhang Jiajia Zeng Shuqun Xu Jianyu Pan Wenzhuo Huang Jianliang Sun Feng Jiang Guangdong provincial key laboratory of chemical Pollution and Environmental Safety&MOE key laboratory of Theoretical Chemistry of Environment School of EnvironmentSouth China Normal UniversityGuangzhou 510006China Guangdong provincial key Lab of Environmental Pollution Control and Remediation technology School of Environmental Science&EngineeringSun Yat-Sen UniversityGuangzhou 510275China

Massive waste aluminum scraps produced from the spent aluminum products have high electron capacity and can be recycled as an attractive alternative to materials based on zerovalent iron(Fe^(0))for the removal of oxidative contaminants from wastewater.This study thus proposed an approach to fabricate micron-sized sulfidated zero-valent iron-aluminum particles(S-Al^(0)@Fe^(0))with high reactivity,electron selectivity and capacity using recycled waste aluminum scraps.S-Al^(0)@Fe^(0)with a three-layer structure contained zero-valent aluminum(Al^(0))core,Fe^(0) middle layer and iron sulfide(FeS)shell.The rates of chromate(Cr(Ⅵ))removal by S-Al^(0)@Fe^(0)at pH 5.0-9.0 were 1.6-5.9 times greater than that by sulfidated zero-valent iron(S-Fe^(0)).The Cr(Ⅵ)removal capacity of S-Al^(0)@Fe^(0)was 8.2-,11.3-and 46.9-fold greater than those of S-Fe0,zero-valent iron-aluminum(Al^(0)-Fe^(0))and Fe^(0),respectively.The chemical cost of S-Al^(0)@Fe^(0) for the equivalent Cr(Ⅵ)removal was 78.5%lower than that of S-Fe^(0).Negligible release of soluble aluminum during the Cr(Ⅵ)removal was observed.The significant enhancement in the reactivity and capacity of S-Al^(0)@Fe^(0)was partially ascribed to the higher reactivity and electron density of the Al0core than Fe^(0).More importantly,S-Al^(0)@Fe^(0) served as an electric cell to harness the persistent and selective electron transfer from the Al^(0)-Fe^(0) core to Cr(Ⅵ)at the surface via coupling Fe^(0)-Fe^(2+)-Fe^(3+)redox cycles,resulting in a higher electron utilization efficiency.Therefore,S-Al^(0)@Fe^(0) fabricated using recycled waste aluminum scraps can be a cost-effective and environmentally-friendly alternative to S-Fe^(0) for the enhanced removal of oxidative contaminants in industrial wastewater.

关键词： Recycled waste aluminum scraps Oxidative contaminants Cr(Ⅵ)reduction Sulfidated Al^(0)@Fe^(0)particle Electron transfer

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Role of methoxy and C_(α)-based substituents in electrochemical oxidation mechanisms and bond cleavage selectivity of β-O-4 lignin model compounds

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Green Energy & Environment 2024年第1期9卷 114-125页

作者： Yang Zhou Qiang Zeng Hongyan He Kejia Wu Fuqiao Liu Xuehui Li School of Chemistry and chemical Engineering The Guangdong Provincial Key Laboratory of Green Chemical Product TechnologyState Key Laboratory of Pulp and Paper EngineeringSouth China University of TechnologyGuangzhouGuangdong510640China CAS key laboratory of Green Process and Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100190China

In order to better understand the specific substituent effects on the electrochemical oxidation process of β-O-4 bond, a series of methoxyphenyl type β-O-4 dimer model compounds with different localized methoxyl groups, including 2-(2-methoxyphenoxy)-1-phenylethanone, 2-(2-methoxyphenoxy)-1-phenylethanol, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanol, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanol have been selected and their electrochemical properties have been studied experimentally by cyclic voltammetry, and FT-IR spectroelectrochemistry. Combining with electrolysis products distribution analysis and density functional theory calculations, oxidation mechanisms of all six model dimers have been explored. In particular, a total effect from substituents of both para-methoxy(on the aryl ring closing to Cα) and Cα-OH on the oxidation mechanisms has been clearly observed, showing a significant selectivity on the Cα-Cβbond cleavage induced by electrochemical oxidations.

关键词： Lignin model compounds β-O-4 dimers Electrochemical oxidation Oxidation mechanisms Substituent effect

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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 batteries.However,commercial polyolefin separators are limited by their poor affinity with electrolytes and low melting points.In 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 performance.In this reinforcedconcrete-like structure,the cellulose is a reinforcing mesh,and the nano-Al_(2)O_(3)acts as concrete to support the separator.After constructing the reinforced-concrete-like structure,the separators exhibit good stability even at 200C(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 performance.Therefore,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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