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Construction of remote cyano-substituted quaternary carbon centers via nickel-catalyzed migratory hydrocyanation of unconjugated dienes

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Science China Chemistry 2024年第10期67卷 3397-3405页

作者： Yidan Xing Rongrong Yu Mingdong Jiao Ting Wang Xianjie Fang Shanghai Key Laboratory for Molecular engineering of Chiral Drugs School of Chemistry and Chemical EngineeringShanghai Jiao Tong University Key Laboratory of Organosilicon Chemistry and material Technology of Ministry of Education Key Laboratory of Organosilicon Material Technology of Zhejiang ProvinceCollege of MaterialChemistry and Chemical EngineeringHangzhou Normal University

The transition-metal-catalyzed migratory functionalization has emerged as a robust protocol for the building of C–C bonds remote from the “initiation” position. However, a similar strategy for the construction of quaternary carbon centers is still underdeveloped and only a limited number of reports exist. Herein, we report a nickel-catalyzed migratory hydrocyanation of unconjugated dienes to construct remote cyano-substituted quaternary carbon centers. This transformation features exceptional regioselectivity, mild reaction conditions, broad substrate scope and high yields. The synthetic utility of this method has been highlighted by a series of product derivatizations, and the potential of this transformation has been extended to synthesize TRPV1 antagonist and the key intermediate in the total synthesis of quebrachamine. Density functional theory(DFT) studies unveiled that the specific catalytic pocket assumed a significant role in the selective formation of cyano-substituted quaternary carbon centers.

关键词： chain-walking regioselectivity remote cyanation quaternary carbon centers unconjugated dienes

Hydrothermal carbonization pretreatment makes a remarkable difference in activation of rice and lettuce in food waste

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Green chemical engineering 2024年第3期5卷 348-363页

作者： Lijun Zhang Yifan Sun Chao Li Shu Zhang Mortaza Gholizadeh Xun Hu School of material Science and engineering University of Jinan Joint International Research Laboratory of Biomass Energy and materials College of Materials Science and Engineering Nanjing Forestry University faculty of chemical and Petroleum engineering University of Tabriz

Cooked rice and the vegetables like lettuce are common kitchen waste, which are carbonaceous materials and have the potential as feedstock for the production of activated carbon. Cooking is similar to hydrothermal treatment（HTC）, which might impact the subsequent activation of kitchen waste. In this study, the HTC of lettuce, rice, or their mixture and the activation of the resulting hydrochars were conducted. The results indicated that cross-polymerization between the N-containing organics from lettuce and the sugar derivatives from rice took place in their co-HTC, which significantly increased the hydrochar yield. Activation of the hydrochar from the coHTC generated the AC with a yield of 2 times that from direct activation of mixed lettuce/rice. However, the coHTC facilitated aromatization, reducing reactivity with K2C2O4in activation and producing the AC with main micropores and low specific surface area. Activation of the hydrochar from HTC of rice followed the above trend,while that from lettuce was the opposite. The organics in lettuce were thermally unstable and could not undergo sufficient aromatization. The activation of hydrochar from HTC of lettuce thus generated the AC with the lowest yield, but the highest specific surface area（1684.9 m2/g）, abundant mesopores, and superior capability for adsorption of tetracycline. However, the environmental impacts and energy consumption for the production of AC from the hydrochar of lettuce were higher than that from hydrochar of co-HTC.

关键词： Food waste Hydrothermal pretreatment Hydrochar chemical activation Products properties

Advanced oxidation via the synergy of C-defective/C-O band modified ultrathin porous g-C3N4 and PMS for efficient photothermal degradation of bisphenol pollutants and lignin derivatives

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Green Energy & Environment 2024年第7期9卷 1159-1170页

作者： Liquan Jing Meng Xie Yuanguo Xu Chun Tong Xia Du Heng Zhao Na Zhong Huaming Li Jinguang Hu School of Chemistry and chemical engineering Jiangsu University Department of chemical and Petroleum engineering University of Calgary School of Pharmacy Jiangsu University School of material Science & chemical engineering Harbin University of Science and Technology Institute for Energy Research Jiangsu University

This work uses thermal polymerization of urea nitrate, oxyacetic acid and urea as the raw material to prepare ultra-thin porous carbon nitride with carbon defects and C-O band（OA-UN-CN）. Density functional theory（DFT） calculations showed OA-UN-CN had narrower band gap,faster electron transport and a new internal construction electric field. Additionally, the prepared OA-UN-CN significantly enhanced photocatalytic activation of peroxymonosulfate（PMS） due to enhanced light absorption performance and faster electron overflow. As the result, the OA-UN-CN/PMS could entirely degrade bisphenol A（BPA） within 30 min, where the photodegradation rate was 81.8 and 7.9 times higher than that of g-C3N4and OA-UN-CN, respectively. Beyond, the OA-UN-CN/PMS could likewise degrade other bisphenol pollutants and sodium lignosulfonate efficiently. We suggested possible photocatalytic degradation pathways accordingly and explored the toxicity of its degradation products. This work provides a new idea on the development of advanced photocatalytic oxidation processes for the treatment of bisphenol pollutants and lignin derivatives, via a metal-free photothermal-catalyst.

关键词： Photothermal-catalytic G-C 3 N 4 Peroxymonosulfate Bisphenol Sodium lignosulfonate

Polyoxometalates-derived ternary metal oxides electrocatalyst for N_(2) reduction under ambient conditions

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Tungsten 2024年第2期6卷 428-437页

作者： Meng-Le Yang Zhong-Xin Jin Xi-Xian Cao Xin-Ming Wang Hui-Yuan Ma Hai-Jun Pang Gui-Xin Yang The School of material Science and chemical engineering Harbin University of Science and TechnologyHarbin 150040China

Accelerating the breaking of the nitrogen nonpolar bond(N≡N)is an important factor to improve the effi ciency of the electro-catalytic nitrogen reduction reaction(e-NRR).In this work,polyoxometalates-derived FeMo-based ternary oxide materials MoO_(2)-Mo_(4)O_(11)-FeMoO_(4)@X(abbreviated as MoFeO@X,X represents the synthesis temperature of 650,750 and 850℃)were designed and synthesized for e-NRR under ambient *** scanning electron microscopy images of MoFeO@750 show an ellipsoidal-like structure(0.86×0.6μm).The relatively large specifi c surface area,formation of multiple interfaces,together with the synergistic eff ect of iron and molybdenum bimetals,would make MoFeO@X catalyst more easily absorb and activate N_(2)in the ***,the synthesized MoFeO@750 shows an optimal NH_(3)production rate of 16.57μg·h^(−1)·mg cat.^(−1)and Faradaic effi ciency of 12.33%at−0.3 V versus reversible hydrogen electrode(ν***),with outstanding electrochemical and structural stability.

关键词： Polyoxometalates Electrocatalytic nitrogen reduction reaction Ternary oxide Electrocatalyst

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Asymmetric copolyimide membranes fabricated by nonsolvent-induced phase separation for He/CH_(4) and He/N_(2) separation

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Frontiers of chemical Science and engineering 2024年第4期18卷 97-106页

作者： Ying Li Lu Wang Junyan Xie Yong Dai Xuehong Gu Xuerui Wang State Key Laboratory of materials-Oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China Quzhou Membrane material Innovation Institute Quzhou 324000China

Membrane gas separation is considered an energy-saving technique to extract He from natural gas due to no phase change and room temperature ***,the membrane performance was strongly limited by the trade-off between permeance and ***,novel 4,4′-(hexafluoroisopropylidene)diphthalic anhydride(6FDA)-2,2′-bis(3-amino-4-hydroxyphenyl)hexafluoropropane(APAF)-5-amino-2-(4-aminobenzene)benzimidazole(BIA)asymmetric membranes with a thickness of 300 nm were successfully prepared by the non-solvent induced phase separation *** membrane performance was modulated by regulating dope solution compositions(e.g.,tetrahydrofuran and polymer concentration).The ideal He/CH_(4) selectivity was 124 and the optimized He permeance reached 87 GPU,beyond the current upper ***/CH_(4) selectivity was 75 and He permeance was 73 GPU for the binary mixture feed containing 0.2 mol%*** membrane showed good resistance to CO_(2) and C_(2)H_(6),which are the typical impurities in natural *** 6FDA-APAF-BIA membranes have good stability(>160 h),which can provide great potential in He extraction from natural gas.

关键词： He separation membrane natural gas copolyimide

Controlled Synthesis of Metal-Nanoparticles Decorated Block Copolymer Hybrid Particles via Emulsion Confined Self-assembly and Their Catalytic Applications

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Chinese Journal of Chemistry 2024年第8期42卷 835-840页

作者： Xiaohua Chang Qunli Yu Dan Ji Yutian Zhu College of material Chemistry and Chemical EngineeringKey Laboratory of Organosilicon Chemistry and Material TechnologyMinistry of EducationHangzhou Normal UniversityHangzhouZhejiang311121 China

Comprehensive Summary Metal nanoparticles(NPs)decorated block copolymer(BCP)hybrid nanoparticles have attracted enormous attention for their actual value in catalysis,medical therapy,and *** confined assembly of BCPs within evaporative emulsion droplet is verified as an effective method to provide polymeric scaffolds to load metal ***,to date,it remains challenging to generate different types of metal NPs decorated BCP hybrid ***,we employed the emulsion confined self-assembly of poly(styrene-b-2-vinylpyridine)(PS-b-P2VP)and the followed seed-mediated growth of Au and palladium(Pd)NPs onto well-defined BCP particles to design a series of Au/Pd decorated BCP hybrid nanoparticles,which exhibited excellent catalytic activity for the reduction of 4-nitrophenol to 4-aminophenol with the reductant of *** work may inspire more researchers to investigate the selective decoration of different metal NPs onto the polymeric scaffolds,broadening the potential applications of the inorganic/organic hybrid nanoparticles.

关键词： Block copolymers Emulsion confined self-assembly Hybrid nanoparticles Catalytic activity Recyclability

Synergistic effect of adsorption and photocatalytic degradation of oilfield-produced water by electrospun photocatalytic fibers of Polystyrene/Nanorod-Graphitic carbon nitride

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Journal of Environmental Sciences 2024年第7期141卷 287-303页

作者： Parisa Azmoon Mehrdad Farhadian Alireza Pendashteh Amir H.Navarchian Department of chemical engineering Faculty of EngineeringUniversity of IsfahanIsfahanIran Department of chemical engineering Faculty of EngineeringUniversity of GuilanRashtIran Department of Water and Environmental engineering Caspian Sea Basin Research CenterUniversity of GuilanRashtIran

Graphitic carbon nitride with nanorod structure(Nr-GCN)was synthesized using melamine as a precursor without any other reagents by hydrothermal pretreatment ***,FTIR,SEM,N_(2)adsorption-desorption from BET,UV-Vis DRS spectroscopy,and photoluminescence were used to characterize the prepared ***,the photoelectrochemical behavior of nanoparticles was studied by photocurrent transient response and cyclic voltammetry ***(PS)fibrous mat was fabricated by electrospinning technique and used as a support for the stabilization of the *** performance of the synthesized nanoparticles and photocatalytic fibers(PS/Nr-GCN)was evaluated in oilfield-produced water treatment under visible light *** this process,oil contaminants were adsorbed by hydrophobic polystyrene fibers and simultaneously degraded by *** removal efficiency of chemical oxygen demand(COD)has been obtained 96.6%and 98.4%by Nr-GCN and PS/Nr-GCN,respectively,at the optimum conditions of pH4,photocatalyst dosage 0.5 g/L,COD initial concentration 550 mg/L,and illumination time 150 *** gas chromatography-mass spectroscopy analysis results showed 99.3%removal of total petroleum hydrocarbons using photocatalytic fibers of PS/*** results demonstrated that the GCN has outstanding features like controllable morphology,visible-light-driven,and showing high potential in oily wastewater ***,the synergistic effect of adsorption and photocatalytic degradation is an effective technique in oilfield-produced water treatment.

关键词： Graphitic carbon nitride(GCN) Nanorod structure Polystyrene fibrous mat Photocatalytic fibers Oilfield-produced water(OPW)

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Stable Cycling of All-Solid-State Lithium Metal Batteries Enabled by Salt engineering of PEO-Based Polymer Electrolytes

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Energy & Environmental materials 2024年第2期7卷 71-78页

作者： Lujuan Liu Tong Wang Li Sun Tinglu Song Hao Yan Chunli Li Daobin Mu Jincheng Zheng Yang Dai Department of chemical engineering Shanghai University School of material Science & engineering Beijing Key Laboratory of Environmental Science and Engineering Beijing Institute of Technology Department of Physics Xiamen University

Poly（ethylene oxide）(PEO)-based polymer electrolytes show the prospect in all-solid-state lithium metal batteries;however,they present limitations of low room-temperature ionic conductivity,and interfacial incompatibility with high voltage ***,a salt engineering of 1,1,2,2,3,3-hexafluoropropane-1,3-disulfonimide lithium salt（LiHFDF）/LiTFSI system was developed in PEO-based electrolyte,demonstrating to effectively regulate Li ion transport and improve the interfacial stability under high *** show,by manipulating the interaction between PEO matrix and TFSI--HFDF-,the optimized solid-state polymer electrolyte achieves maximum Li+conduction of 1.24×10-4S cm-1at 40℃,which is almost 3 times of the ***,the optimized polymer electrolyte demonstrates outstanding stable cycling in the LiFePO4/Li and LiNi0.8Mn0.1Co0.1O2/Li（3.0-4.4 V,200 cycles） based all-solid-state lithium batteries at 40℃.

关键词： all-solid-state battery high voltage li-ion conductivity molecular interaction poly(ethylene oxide)

Advances in noble metal-modified g-C3N4 heterostructures toward enhanced photocatalytic redox ability

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International Journal of Minerals,Metallurgy and materials 2024年第11期 2368-2389页

作者： Xiao Zhang Ping Yang faculty of chemical engineering and Technology Cracow University of Technology School of material Science&engineering University of Jinan

The photocatalytic activity of catalysts depends on the energy-harvesting ability and the separation or transport of photogenerated carriers. The light absorption capacity of graphitic carbon nitride（g-C3N4）-based composites can be enhanced by adjusting the surface plasmon resonance（SPR） of noble metal nanoparticles（e.g., Cu, Au, and Pd） in the entire visible region. Adjustments can be carried out by varying the nanocomponents of the materials. The SPR of noble metals can enhance the local electromagnetic field and improve interband transition, and resonant energy transfer occurs from plasmonic dipoles to electron–hole pairs via near-field electromagnetic interactions. Thus, noble metals have emerged as relevant nanocomponents for g-C3N4used in CO2photoreduction and water ***, recent key advances in noble metals（either in single atom, cluster, or nanoparticle forms） and composite photocatalysts based on inorganic or organic nanocomponent-incorporated g-C3N4nanosheets are systematically discussed, including the applications of these photocatalysts, which exhibit improved photoinduced charge mobility in CO2photoconversion and H2production. Issues related to the different types of multi-nanocomponent heterostructures（involving Schottky junctions, Z-/S-scheme heterostructures, noble metals, and additional semiconductor nanocomponents） and the adjustment of dimensionality of heterostructures（by incorporating noble metal nanoplates on g-C3N4forming 2D/2D heterostructures） are explored. The current prospects and possible challenges of g-C3N4composite photocatalysts incorporated with noble metals（e.g., Au, Pt, Pd, and Cu）, particularly in water splitting, CO2reduction, pollution degradation,and chemical conversion applications, are summarized.

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