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Highly efficient catalyzed by imidazolium-based dual-sulfonic acid functionalized ionic liquids for liquid phase Beckmann rearrangement:experiments and COSMO-RS calculations

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Green Chemical Engineering 2024年第1期5卷 108-118页

作者： Xin Guo zhiyuan wang Ye Yang Jiahui zhang Yanduo Liu zhiyuan Mu Siqi Jiang Chunxiao Ren Dan Lv yufeng Hu Zhichang Liu State Key Laboratory of Heavy Oil Processing and High Pressure Fluid Phase Behavior&Property Research Laboratory China University of PetroleumBeijing102249China School of Chemistry and Materials Science University of Science and Technology of ChinaHefei230026China School of Light Industry and Engineering South China University of TechnologyGuangzhou510641China

A production technique with the high yield and environmentally friendly process need be developed forε-Caprolactam(CPL)in the chemical *** technology is highly desired to design and synthesize high--performance catalysts for liquid phase Beckmann rearrangement of cyclohexanone oxime(CHO)to *** this work,3-methyl-1-(propyl-4-sulfonyl)imidazolium methanesulfonate([PHSO_(3)MIM][MSA])with highly efficient and excellent yield is synthesized *** the optimum molar ratio of ZnCl_(2)over[PHSO_(3)MIM][MSA]was 0.02,it exhibits the high selectivity(94%)of CPL at 90℃for 1 ***,Fourier-transform infrared(FT-IR)investigations show that the functional Br∅nsted-Lewis acidic types of ionic liquids(ILs)are formed by the uniformly distributed ZnCl_(2)and[PHSO_(3)MIM][MSA].In addition,the hydrogen bond(H-bond)is formed between CHO and *** ten reaction cycles,no significant structure changes are observed in the recovered[PHSO_(3)MIM][MSA]-ZnCl_(2).The solubilities of ILs are predicted by using COSMO-RS model,the results show that[PHSO_(3)MIM][MSA]is a promising candidate for the liquid phase Beckmann rearrangement of CHO into ***,a theoretical model of the H-bond interactions between ILs and CHO is further confirmed to support the advance of reaction mechanism.A feasible way is provided for the CPL production technique in the liquid phase Beckmann rearrangement reaction.

关键词： Liquid phase Beckmann rearrangement Imidazolium-based ionic liquids COSMO-RS calculations H-bond

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Monolithic integrated optoelectronic chip for vector force detection

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Microsystems & Nanoengineering 2024年第3期10卷 245-257页

作者： Jiansong Feng Zhongqi wang Mengyuan zhanghu Xu zhang Yong Shen Jing Yang zhibin Li Bin Chen Taihong wang Xiaolong Chen Zhaojun Liu Department of Electrical and Electronic Engineering Southern University of Science and TechnologyShenzhen 518055China Department of Electrical and Electronic Engineering The University of Hong KongHong KongChina

Sensors with a small footprint and real-time detection capabilities are crucial in robotic surgery and smart wearable *** device footprint while maintaining its high performance is a major challenge and a significant limitation to their ***,we proposed a monolithic integrated micro-scale sensor,which can be used for vector force *** sensor combines an optical source,four photodetectors,and a hemispherical silicone elastomer component on the same sapphire-based AlGaInP *** chip-scale optical coupling is achieved by employing the laser lift-off techniques and the flip-chip bonding to a processed sapphire *** hemispherical structure device can detect normal and shear forces as low as 1mN within a measurement range of 0–220 mN for normal force and 0–15 mN for shear *** packaging,the sensor is capable of detecting forces over a broader range,with measurement capabilities extending up to 10 N for normal forces and 0.2 N for shear *** has an accuracy of detecting a minimum normal force of 25 mN and a minimum shear force of 20 ***,this sensor has been validated to have a compact footprint of approximately 1.5 mm^(2),while maintaining high real-time *** also demonstrate its promising potential by combining this sensor with fine surface texture perception in the fields of compact medical robot interaction and wearable devices.

关键词： robot force smart

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UDP-glucosyltransferase 71C4 controls the flux of phenylpropanoid metabolism to shape cotton seed development

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Plant Communications 2024年第8期5卷 157-171页

作者： Yiwen Cao Zegang Han zhiyuan zhang Lu He Chujun huang Jinwen Chen Fan Dai Lisha Xuan Sunyi Yan Zhanfeng Si Yan Hu Tianzhen zhang Zhejiang Provincial Key Laboratory of Crop Genetic Resources the Advanced Seed InstitutePlant Precision Breeding AcademyCollege of Agriculture and BiotechnologyZhejiang UniversityHangzhouChina Hainan Institute Zhejiang UniversitySanyaChina

Seeds play a crucial role in plant reproduction,making it essential to identify genes that affect seed devel*** this study,we focused on UDP-glucosyltransferase 71C4(UGT71C4)in cotton,a member of the glycosyltransferase family that shapes seed width and length,thereby influencing seed index and seed cotton *** of UGT71C4 results in seed enlargement owing to its glycosyltransferase activity on flavonoids,which redirects metabolic flux from lignin to flavonoid *** shift promotes cell proliferation in the ovule via accumulation of flavonoid glycosides,significantly enhancing seed cotton yield and increasing the seed index from 10.66 g to 11.91 *** contrast,knockout of UGT71C4 leads to smaller seeds through activation of the lignin metabolism pathway and redirection of metabolic flux back to lignin *** redirection leads to increased ectopic lignin deposition in the ovule,inhibiting ovule growth and development,and alters yield components,increasing the lint percentage from 41.42%to 43.40%and reducing the seed index from 10.66 g to 8.60 *** research sheds new light on seed size development and reveals potential pathways for enhancing seed yield.

关键词： UDP-glucosyltransferase seed development phenylpropanoid metabolism gene editing

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Comparative study on the hydrogen storage performance of as-milled MgRENi rapid quenched alloy catalyzed by metal sulfides

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Journal of Magnesium and Alloys 2024年第5期12卷 2010-2023页

作者： Xiaoping Dong Zhaoqing zhang Liying Yang Shenghai Xin Dandan Su zhiyuan Li Department of Mechanical Design and Manufacture and Automation Hebei UniversityBaoding 071000PR China Baoding New Energy Vehicle Power Engineering Technology Research Center Hebei UniversityBaoding 071002PR China Hebei Technology Innovation Center for Lightweight of New Energy Vehicle Power System(Preparation) Hebei UniversityBaoding 071002PR China

The composites of Mg_(20)Pr_(1)Sm_(3)Y_(1)Ni_(10)as-quenched alloy and 3 wt.%M(M=CoS,CoS_(2),MoS_(2))catalyst were prepared by high-speed vibration ball *** effects of metal sulfides on the hydrogenation and dehydrogenation dynamics of alloys were *** results show that the as-milled composites contain a large number of amorphous embedded by a small amount of nanocrystals,and there are many point *** ball milling,the crystal grain size in the composites containing CoS is relatively larger,followed by CoS_(2)and MoS_(2)*** hydrogenation,the amorphous phase is crystallized to form Mg_(2)NiH_(4),YH_(3),Pr_(8)H_(18.96),Sm_(3)H_7,Mg,Co or Mo phases,however,Mg_(2)Ni,YH_(2),PrH_(2)and Ni_(3)Y phases appeared after *** maximum hydrogenation capacity of the composites containing CoS,CoS_(2)and MoS_(2)are 3.939,4.265 and 4.507 wt.%,*** hydrogenation saturation ratio of composite containing MoS_(2)is higher than that of the composites containing CoS and CoS_(2).The dehydrogenation activation energy of the composites containing CoS,CoS_(2)and MoS_(2)is 107.76,68.43 and 63.28 ***^(-1).H_(2).On the improvement of hydrogen storage performance of Mg_(20)Pr_(1)Sm_(3)Y_(1)Ni_(10)alloy,the catalytic effect of MoS_(2)sulfide is better than that of CoS_(2)sulfide,and which is better than CoS sulfide.

关键词： Mg_(20)Pr_(1)Sm_(3)Y_(1)Ni_(10)as-quenched alloy CoS CoS_(2)and MoS_(2)sulfide Milling Activation energy Hydrogen storage dynamics

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Synergistic effect of homojunction and Ohmic junctions in CdS boosting spatial charge separation for U(VI)photoreduction

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Nano Research 2024年第8期17卷 6849-6859页

作者： Haonan Pei Zhimin Dong Zifan Li Jian huang yuanping Jiang Zuojia Li Lin Xu Xiaohong Cao yunhai Liu zhibin zhang Guoping Yang State Key Laboratory of Nuclear Resources and Environment East China University of TechnologyNanchang 330013China

Photo-excited holes usually migrate to the surface of the catalyst and rapidly recombine with electrons,reducing the photocatalytic reduction efficiency of uranium(VI)(U(VI))in radioactive ***,we employed a straightforward synthesis technique to meticulously shape and manipulate the morphology of CdS to precisely construct CdS-Ni dandelion-like composites with different aspect ***,the introduction of crystal facet homojunction with Ohmic contacts in this unique morphology siqnificantly improves the photocatalytic ***-dependent photoluminescence spectroscopy(TD-PL)verifies that the composite material positively effects on the dissociation of *** 30 min,CdS(002)/(102)/Ni-4 removed 98% of the uranium content in solution and showed a rather high apparent rate constant(0.114 min^(−1)),which was 4.8 times higher than that of CdS nanospheres(NSs)(0.024 min^(−1))and 3.7 times higher than that of CdS nanorods(NRs)(0.031 min^(−1)).This is much higher the most reported photocatalysts for U(VI)*** after 5 consecutive cycles,the photocatalytic efficiency only decreased by 7%.This offers a fresh perspective on constructing a new perspective for building a green,efficient,and multi mechanism collaborative catalytic system to remediate environmental pollution.

关键词： uranium dandelion-shaped axial size effect crystal facet homojunction ohmic contact

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FUT8-mediated aberrant N-glycosylation of SEMA7A promotes head and neck squamous cell carcinoma progression

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International Journal of Oral Science 2024年第2期16卷 333-348页

作者： Zhonglong Liu Xiaoyan Meng yuxin zhang Jingjing Sun Xiao Tang zhiyuan zhang Liu Liu yue He Department of Oral Maxillofacial&Head and Neck Oncology Shanghai Ninth People’s Hospital Affiliated to Shanghai Jiao Tong University School of MedicineNational Clinical Research Center for Oral DiseaseShanghaiChina Department of Oral Surgery Shanghai Ninth People’s HospitalShanghai Jiao Tong University School of MedicineCollege of StomatologyShanghai Jiao Tong UniversityNational Center for StomatologyNational Clinical Research Center for Oral DiseasesShanghaiChina Department of Oral Pathology Shanghai Ninth People’s Hospital Affiliated to Shanghai Jiao Tong University School of MedicineNational Clinical Research Center for Oral Disease ShanghaiShanghaiChina

SEMA7A belongs to the Semaphorin family and is involved in the oncogenesis and tumor *** glycosylation has been intricately linked with immune escape and tumor ***7A is a highly glycosylated protein with five glycosylated *** underlying mechanisms of SEMA7A glycosylation and its contribution to immunosuppression and tumorigenesis are ***,we identify overexpression and aberrant N-glycosylation of SEMA7A in head and neck squamous cell carcinoma,and elucidate fucosyltransferase FUT8 catalyzes aberrant core fucosylation in SEMA7A at N-linked oligosaccharides(Asn 105,157,258,330,and 602)via a direct protein‒protein interaction.A glycosylated statue of SEMA7A is necessary for its intra-cellular trafficking from the cytoplasm to the *** EGF triggers SEMA7A N-glycosylation through increasing the binding affinity of SEMA7A toward FUT8,whereas TGF-β1 promotes abnormal glycosylation of SEMA7A via induction of epithelial–mesenchymal *** N-glycosylation of SEMA7A leads to the differentiation of CD8^(+)T cells along a trajectory toward an exhausted state,thus shaping an immunosuppressive microenvironment and being resistant immunogenic cell *** of SEMA7A significantly improves the clinical outcome of EGFR-targeted and anti-PD-L1-based ***,we also define RBM4,a splice regulator,as a downstream effector of glycosylated SEMA7A and a pivotal mediator of PD-L1 alternative *** findings suggest that targeting FUT8-SEMA7A axis might be a promising strategy for improving antitumor responses in head and neck squamous cell carcinoma patients.

关键词： aberrant squamous SEMA

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Yangtze River Delta Aerosol liquid water in PM_(2.5)and its roles in secondary aerosol formation at a regional site of Yangtze River Delta

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Journal of Environmental Sciences 2024年第4期138卷 684-696页

作者： Ruifang Shi Fei zhang Yemin Shen Jiasi Shen Bingye Xu Binyu Kuang Zhengning Xu Lingling Jin Qian Tang Xudong Tian zhibin wang College of Environmental and Resource Sciences Zhejiang Provincial Key Laboratory of Organic Pollution Process and ControlZhejiang UniversityHangzhou 310058China ZJU-Hangzhou Global Scientific and Technological Innovation Center Zhejiang UniversityHangzhou 311215China Zhejiang Ecological and Environmental Monitoring Center Hangzhou 310012China

Aerosol liquid water content(ALWC)plays an important role in secondary aerosol *** this study,a whole year field campaign was conducted at Shanxi in north Zhejiang Province during *** estimated by ISORROPIA-Ⅱ was then investigated to explore its characteristics and relationship with secondary *** exhibited a highest value in spring(66.38μg/m^(3)),followed by winter(45.08μg/m^(3)),summer(41.64μg/m^(3)),and autumn(35.01μg/m^(3)),*** was supposed that the secondary inorganic aerosols(SIA)were facilitated under higher ALWC conditions(RH>80%),while the secondary organic species tended to form under lower ALWC *** RH(>80%)promoted the NO_(3)^(-)formation via gas-particle partitioning,while SO_(4)^(2-)was generated at a relative lower RH(>50%).The ALWC was more sensitive to NO_(3)^(-)(R=0.94)than SO_(4)^(2-)(R=0.90).Thus,the self-amplifying processes between the ALWC and SIA enhanced the particle mass *** sensitivity of ALWC and OX(NO_(2)+O_(3))to secondary organic carbon(SOC)varied in different seasons at Shanxi,more sensitive to aqueous-phase reactions(daytime R=0.84;nighttime R=0.54)than photochemical oxidation(daytime R=0.23;nighttime R=0.41)in wintertime with a high level of OX(daytime:130-140μg/m^(3);nighttime:100-140μg/m^(3)).The self-amplifying process of ALWC and SIA and the aqueous-phase formation of SOC will enhance aerosol formation,contributing to air pollution and reduction of visibility.

关键词： Aerosol liquid water content Nitrate Sulfate Secondary organic compounds Aqueous-phase reaction

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Photocatalytic degradation of methylene blue over MIL-100(Fe)/GO composites: a performance and kinetic study

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International Journal of Coal Science & Technology 2024年第3期11卷 208-222页

作者： yuxue Wei zhiyuan Fu Yingzi Meng Chun Li Fu Yin Xue wang Chenghua zhang Lisheng Guo Song Sun School of Chemistry and Chemical Engineering Anhui UniversityHefei230601AnhuiChina Anhui Tanxin Technology Co. LtdHuaibei235141AnhuiChina

Adsorption coupled with photocatalytic degradation is proposed to fulfill the removal and thorough elimination of organic ***,we report a facile hydrothermal synthesis of MIL-100(Fe)/GO *** adsorption and photocatalytic degradation process of methylene blue(MB)on MIL‐100(Fe)/GO composites were systematically studied from performance and kinetic perspectives.A possible adsorption‐photocatalytic degradation mechanism is *** optimized 1M8G composite achieves 95%MB removal(60.8 mg/g)in 210 min and displays well recyclability over ten *** obtained MB adsorption and degradation results are well fitted onto Langmuir isotherm and pseudo‐second order kinetic *** study shed light on the design of MOFs based composites for water treatment.

关键词： Graphene oxide Metal organic frameworks Methylene blue Adsorption Photocatalytic degradation

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Highly efficient electrosynthesis of H_(2)O_(2)in acidic electrolyte on metal-free heteroatoms co-doped carbon nanosheets and simultaneously promoting Fenton process

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Chinese Chemical Letters 2024年第7期35卷 514-518页

作者： Xiaodan wang Yingnan Liu zhibin Liu Zhongjian Li Tao zhang Yi Cheng Lecheng Lei Bin Yang Yang Hou Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310058China Institute of Zhejiang University-Quzhou Quzhou 324000China Donghai Laboratory Zhoushan 316000China Ningbo Institute of Materials Technology&Engineering University of Chinese Academy of SciencesNingbo 315200China School of Biological and Chemical Engineering NingboTech UniversityNingbo 315100China Zhejiang Hengyi Petrochemical Research Institute Co. Ltd.Hangzhou 310058China

Recently electrochemical synthesis of H_(2)O_(2)through oxygen reduction reaction(ORR)via 2e^(-)pathway is considered as a green and on-site ***,it still remains a big challenge for fabricating novel metal-free catalysts under acidic solutions,since it suffers from high overpotential due to the intrinsically week*OOH ***,a co-doped carbon nanosheet(O/N–C)catalyst toward regulating O and N content was synthesized for improving the selectivity and activity of H_(2)O_(2)electrosynthesis *** O/N–C exhibits outstanding 2e-ORR performance with low onset potential of 0.4 V(***)and a selectivity of 92.4%in 0.1 mol/L HClO_(4)*** in situ electrochemical impedance spectroscopy(EIS)tests reveals that the N incorporation contributes to the fast ORR *** density functional theory(DFT)calculations demonstrate that the binding strength of*OOH was optimized by the co-doping of oxygen and nitrogen at certain content,and the O/N–C–COOH site exhibits a lower theoretical overpotential for H_(2)O_(2)formation than O–C–COOH ***,the promoted kinetics for typical organic dye degradation in simultaneous electron-Fenton process on O/N–C catalyst was demonstrated particularly for broadening its environmental application.

关键词： Oxygen reduction Metal-free catalyst H_(2)O_(2)electrosynthesis N doping Carbon materials

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Descriptor-augmented machine learning for enzyme-chemical interaction predictions

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Synthetic and Systems Biotechnology 2024年第2期9卷 259-268页

作者： Yilei Han Haoye zhang Zheni Zeng zhiyuan Liu Diannan Lu Zheng Liu Department of Chemical Engineering Tsinghua UniversityBeijing100084China Department of Computer Science and Technology Tsinghua UniversityBeijing100084China

Descriptors play a pivotal role in enzyme design for the greener synthesis of biochemicals,as they could characterize enzymes and chemicals from the physicochemical and evolutionary *** study examined the effects of various descriptors on the performance of Random Forest model used for enzyme-chemical relationships *** curated activity data of seven specific enzyme families from the literature and developed the pipeline for evaluation the machine learning model performance using 10-fold *** influence of protein and chemical descriptors was assessed in three scenarios,which were predicting the activity of unknown relations between known enzymes and known chemicals(new relationship evaluation),predicting the activity of novel enzymes on known chemicals(new enzyme evaluation),and predicting the activity of new chemicals on known enzymes(new chemical evaluation).The results showed that protein descriptors significantly enhanced the classification performance of model on new enzyme evaluation in three out of the seven datasets with the greatest number of enzymes,whereas chemical descriptors appear no effect.A variety of sequence-based and structure-based protein descriptors were constructed,among which the esm-2 descriptor achieved the best *** enzyme families as labels showed that descriptors could cluster proteins well,which could explain the contributions of descriptors to the machine learning *** a counterpart,in the new chemical evaluation,chemical descriptors made significant improvement in four out of the seven datasets,while protein descriptors appear no *** attempted to evaluate the generalization ability of the model by correlating the statistics of the datasets with the performance of the *** results showed that datasets with higher sequence similarity were more likely to get better results in the new enzyme evaluation and datasets with more enzymes were more likely beneficial from the protein

关键词： Enzyme-substrate interaction Enzyme design Machine learning Descriptor

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