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Low-content Pt-triggered the optimized d-band center of Rh metallene for energy-saving hydrogen production coupled with hydrazine degradation

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Journal of Energy Chemistry 2023年第10期85卷 58-66,I0004页

作者： Qiqi Mao Wenxin Wang Kai Deng Hongjie Yu Ziqiang Wang You Xu Xiaonian Li Liang Wang Hongjing Wang State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology College of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014ZhejiangChina

Utilizing the hydrazine-assisted water electrolysis for energy-efficient hydrogen production shows a promising application, which relies on the development and design of efficient bifunctional electrocatalysts. Herein, we reported a low-content Pt-doped Rh metallene(Pt-Rhene) for hydrazine-assisted water electrolysis towards energy-saving hydrogen(H_(2)) production, where the ultrathin metallene is constructed to provide enough favorable active sites for catalysis and improve atom ***, the synergistic effect between Rh and Pt can optimize the electronic structure of Rh for improving the intrinsic activity. Therefore, the required overpotential of Pt-Rhene is only 37 mV to reach a current density of-10 mA cm^(-2) in the hydrogen evolution reaction(HER), and the Pt-Rhene exhibits a required overpotential of only 11 mV to reach a current density of 10 mA cm^(-2) in the hydrazine oxidation reaction(HzOR). With the constructed HER-HzOR two-electrode system, the Pt-Rhene electrodes exhibit an extremely low voltage(0.06/0.19/0.28 V) to achieve current densities of 10/50/100 mA cm^(-2) for energy-saving H_(2) production, which greatly reduces the electrolysis energy consumption. Moreover,DFT calculations further demonstrate that the introduction of Pt modulates the electronic structure of Rh and optimizes the d-band center, thus enhancing the adsorption and desorption of reactant/intermediates in the electrocatalytic reaction.

关键词： Pt-Rhene Synergistic effect Hydrogen evolution reaction Hydrazine oxidation reaction Energy-saving H_(2)production

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Mechanistic insights into propylene oxidation to acrolein over gold catalysts

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Chinese Journal of chemical engineering 2023年第5期57卷 39-49页

作者： Bin Lin Wenyao Chen Nan Song Zhihua Zhang Qianhong Wang Wei Du Xinggui Zhou Xuezhi Duan State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China

Direct epoxidation of propylene with H_(2)/O_(2),being the dream reaction for propylene oxide(PO)production,has raised wide scientific and industrial *** understanding the formation mechanism of acrolein,as the main by-product of this epoxidation process,is very important to achieve the high yield of *** this study,we perform the spin-polarized density functional theory(DFT)calculations to investigate the reaction pathway from propylene to acrolein over two representative Au surfaces,that is,Au(111)and Au(100),which incorporates propylene adsorption,methyl hydrogen activation and acrolein *** results show that the oxygenated species(mainly O^(*),OH^(*)and OOH^(*))are able to stabilize the adsorption of propylene to decrease the energy barrier for its *** is demonstrated that the OOH^(*)on Au(111)surface emerges as the most easily formed oxygenated species via the H-assisted O_(2) dissociation,which is also the most active for the cleavage of methyl CAH bond in ***,three pathways of acrolein formation activated by O^(*)/OH^(*)/OOH^(*)are analyzed,in which O^(*)is found as the key species to form ***,Bader charge analysis was conducted to explore the reasons behind the promotion effect of the oxygenated *** insights reported here could be valuable in the design and optimization of gold catalysts for the direct epoxidation of propylene.

关键词： Acrolein formation Oxygenated species DFT calculations Au surfaces Reaction mechanism

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Phosphotungstic acid immobilized on amino-functionalized TS-1 zeolite as a solid acid catalyst for the synthesis of tributyl citrate

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Chinese Journal of chemical engineering 2024年第6期70卷 199-210页

作者： Pei Li Bianfang Shi Junyao Shen Ran Cui Wenze Guo Ling Zhao Zhenhao Xi State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China Key Laboratory of Smart Manufacturing in Energy Chemical Process Ministry of EducationEast China University of Science and TechnologyShanghai 200237China

The amino-functionalization of TS-1 zeolite followed by immobilization of phosphotungstic acid(HPW)was presented to prepare a strong solid acid catalyst for the synthesis of bio-based tributyl citrate from the esterification of citric acid and n-butanol.γ-Aminopropyltriethoxysilane(APTES)was first grafted on the TS-1 zeolite via the condensation reactions with surface hydroxyl groups,and subsequently the HPW was immobilized via the reaction between the amino groups and the protons from HPW-forming strong ionic *** Keggin structure of HPW and MFI topology of TS-1 zeolite were well maintained after the *** amino-functionalization generated abundant uniformly distributed active sites on TS-1 for HPW immobilization,which promoted the dispersity,abundance,as well as the stability of the acid *** tetrahedrally coordinated framework titanium and non-framework titania behaved as weak Lewis acid sites,and the protons from the immobilized HPW acted as the moderate or strong Brønsted acid *** optimized TBC yield of 96.2%(mol)with a conversion of-COOH of 98.1%(mol)was achieved at 150℃for 6 h over the HPW immobilized on amino-functionalized *** catalyst exhibited good stability after four consecutive reaction runs,where the activity leveled off at still a relatively high level after somewhat deactivation possibly caused by the leaching of a small portion of weakly anchored APTES or HPW.

关键词： Amino-functionalization Phosphotungstic acid TS-1 zeolite Esterification Tributyl citrate

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Designing high-area-loading lithium metal batteries with in-situ polymerized electrolyte featuring gradient molar mass

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Journal of Energy Chemistry 2025年第4期103卷 383-392页

作者： Mengjun Sun Zhi Wang Zhe Sheng Xiang Zhen Juhui Jiang Xiaobing Wang Jia Xie School of Chemistry and Chemical Engineering Henan Normal UniversityXinxiang 453007HenanChina State Key Laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina

In-situ polymerized solid-state lithium metal batteries have garnered significant attention due to their conformal interface contact and continuous pathways for lithium ion(Li^(+))***,their electrochemical performance is often hindered by slow Li^(+)transport within high-area-loading *** study presents an in-situ poly(ε-caprolactone)electrolyte with gradient molar mass(iGPCE)through lithium metal anode(LMA)-induced anionic ring-opening *** electrochemical and kinetic analyses reveal that the iGPCE,characterized by low molar mass(M),significantly enhances Li~+diffusion within high-area-loading cathodes and bulk electrolytes,thereby reducing concentration polarization and promoting uniform electrochemical ***,the high M region on LMA side acts as artificial solid electrolyte interphases,stabilizing the stripping and plating of ***,Li//LFP(20 mg cm^(-2))and Li//NCM622(7.4 mg cm^(-2))utilizing iGPCE exhibit stable charge/discharge *** study offers a fresh approach to accelerate Li~+diffusion kinetics of high-area-loading batteries and suggests broad applicability in other systems.

关键词： Gradient molar mass High-area-loading cathode In-situ polymerization Fast Li^(+)transport kinetics Lithium metal batteries

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Rapid Self-healing and Strong Adhesive Elastomer via Supramolecular Aggregates from Core-shell Micelles of Silicon Hydroxyl-functionalized cis-Polybutadiene

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Chinese Journal of Polymer Science 2023年第1期41卷 84-94页

作者： Ying-Ying Zheng Han Zhu Yi Tan Feng-Yi-Qi Liu Yi-Xian Wu State Key Laboratory of Chemical Resource Engineering Beijing Advanced innovation Center for Soft Matter Science and EngineeringBeijing University of Chemical TechnologyBeijing100029China

Liquid trimethoxy silane-functionalized cis-polybutadiene(cis-PB-Si(OMe)3),possessing number-average molecular weights of cis-PB segments(Mn,PB)ranging from 1800 g/mol to 5400 g/mol,with cis-1,4 content of ca.80%and high functionality(>96%)could be synthesized by coordination copolymerization of living cis-PB chain ends with ethenyltrimethoxy-silane with neodymium-based catalytic *** silicon hydroxyl-functionalized cis-polybutadiene(cis-PB-Si(OH)_(3))-based micelles in water have been achieved by in situ hydrolysis of cis-PB-Si(OMe)_(3)in hexane/water mixture(pH=6.8)at 70℃and by sequential removal of residue *** size of the above micelles with soft elastic cis-PB cores could be remarkably enlarged by loading SiO_(2)nanoparticles on their surfaces via hydrogen bonding *** supramolecular long chain aggregates or networks formed by hydrogen bonding interaction and possible O—Si—O chemical bonds between cis-PB-Si(OH)3-based micellar surfaces had relatively large size and thus precipitated from water after several months of storage,leading to production of cis-PB-Si(OH)_(3)solid elastomer with extremely low T_(g)at−107.0℃.The left cis-PB-Si(OH)_(3)-based micelles in water with relatively small size gradually formed the water-insoluble cis-PB-Si(OH)_(3)-based supramolecular aggregates or *** cis-PB-Si(OH)_(3)-based supramolecular elastomer exhibited excellent self-healing property within 60 s at 25℃.The elastomer(20 mg)in a joint of 25 mm×30 mm(2.7 mg/cm^(2))provided very strong adhesion for two pieces of glass and the bound glass keep unchanged at room temperature for 98 h even hung with 100 g of steel column *** cis-PB-Si(OH)3-based supramolecular elastomer would have potential applications in adhesives,self-healing materials,damping materials and elastic materials.

关键词： Amphiphilicity Polybutadiene Core-shell micelles Supramolecular aggregates

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Rapid evaluating caking tendency of nonspherical crystals by developing a shape-based crystal bridge growth model

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Particuology 2024年第12期95卷 265-278页

作者： Mingxuan Li Mengdi Zhang Wei Zhao Leida Zhang Mingyang Chen Dandan Han Junbo Gong State Key Laboratory of Chemical Engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China Institute of Shaoxing Tianjin UniversityShaoxing312300China Shandong Fuyang Biotechnology Co. Ltd.Dezhou253100China

Crystal caking is a decisive factor affecting the quality of high-end fine chemicals,whereas lack of shape-to-caking understanding results in considerable waste of time,severely delaying high-end fine chemical *** this basis,a morphology-based caking evaluation model is developed with 74%and 96%time savings compared to previous modeling and non-modeling experiments,respectively,while guaranteeing superior *** crystal morphology is expressed as a function of the aspect ratio and the particle size *** quantitative relationships between these parameters and the caking tendency are deduced,firstly achieving morphology anti-caking criterion *** D-allulose crystals,considering humidity,and particle size,an aspect ratio is below 3 is the standard for combating caking,which has not been reported ***,the specific effect of crystal morphology on caking behavior is quantitatively *** knowledge obtained can be applied to rapidly and quantitatively design anti-caking storage systems for products in warehouses.

关键词： Caking evaluation Crystal morphology D-allulose Rod-like crystal Crystal bridge growth model

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An innovative graphene-based phase change composite constructed by syneresis with high thermal conductivity for efficient solar-thermal conversion and storage

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Journal of Materials Science & technology 2024年第11期178卷 179-187页

作者： Jianqiang Wang Weijie Li Xinya Zhang School of Chemistry and Chemical Engineering Guangdong Provincial Key Lab of Green Chemical Product TechnologySouth China University of TechnologyGuangzhou 510640China

Graphene-based phase change composites hold significant potential for solar energy utilization,but their poor thermal conductivity hinders their practical *** this work,an air-dried graphene skele-ton(AGS)with excellent thermal conductivity enhancement efficiency was constructed by the ice tem-plating method and syneresis,and the air-dried graphene phase change composite(AGP)was subse-quently obtained through vacuum-impregnating n-Docosane(C22)into *** syneresis effectively re-duced the phonon scattering between graphene sheets within AGS and increased the density of AGS to 0.1701 g/***,with a graphene skeleton loading of 23.82 wt.%,AGP exhibited excellent thermal conductivity of 9.867 W/(m K),outstanding electrical conductivity of 68.08 S/cm,and remarkable shape ***,AGP demonstrated a melting enthalpy of 188.5 J/g and an outstanding solar-thermal conversion efficiency of 93.98%,showing enormous potential for the utilization of solar energy.

关键词： Syneresis Graphene skeletons Thermal conductivities Phase change composites Solar-thermal conversion

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Electrochemical reconstruction: a new perspective on Sn metal-organic complex microbelts as robust anode for lithium storage

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Rare Metals 2024年第1期43卷 76-86页

作者： Jin-Ke Shen Nai-Teng Wu Li-Yuan Wang Gang Jiang Dong-Lei Guo Jin Li Gui-Long Liu Hong-Yu Mi Huan Pang Xian-Ming Liu Key Laboratory of Function-oriented Porous Materials of Henan Province College of Chemistry and Chemical EngineeringLuoyang Normal UniversityLuoyang 471934China State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources School of Chemical Engineering and TechnologyXinjiang UniversityUrumqi 830046China School of Chemistry and Chemical Engineering Institute for Innovative Materials and EnergyYangzhou UniversityYangzhou 225009JiangsuChina

Tin-based materials with high theoretical capacity and suitable working voltage are ideal anode materials for lithium-ion batteries(LIBs). However, to overcome their shortcomings(volume expansion and inferior stability), the preparation processes are usually complicated and expensive. Herein, a tin-based metal-organic complex(tin 1,2-benzenedicarboxylic acid, Sn-BDC)with one-dimensional microbelt morphology is synthesized by a facile, rapid and low-cost co-precipitation method, and served as anode material for LIBs without any post-treatment. Sn-BDC exhibits a high reversible capacity with609/440 m Ah·g^(-1) at 50/2000 m A·g^(-1), and robust cycling stability of 856 m Ah·g^(-1) after 200 cycles at 200 m A·g^(-1),which are obviously superior to that of the Sn Ox/C counterparts. Moreover, an electrochemical reconstruction perspective on the lithium storage mechanism of Sn-BDC is proposed by systematic ex-situ characterizations. The reconstructed SnO_(2) replaces Sn-BDC and becomes the active material in the subsequent cycles. As the by-product of the lithiation reaction, the formed Li-based metal-organic complex(Li-BDC, wrapped around the reconstructed SnO_(2)) plays an important role in alleviating volume expansion and accelerating the charge transfer *** work is beneficial to design and construct the new electrode materials based on the electrochemical reconstruction for advanced LIBs.

关键词： Electrochemical reconstruction Metal-organic complex Anode Lithium storage mechanism Lithium-ion batteries

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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 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 UniversityHangzhou 311121China Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China

The transition-metal-catalyzed migratory functionalization has emerged as a robust protocol for the building of C–C bonds remote from the“initiation”***,a similar strategy for the construction of quaternary carbon centers is still underdeveloped and only a limited number of reports ***,we report a nickel-catalyzed migratory hydrocyanation of unconjugated dienes to construct remote cyano-substituted quaternary carbon *** transformation features exceptional regioselectivity,mild reaction conditions,broad substrate scope and high *** 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 *** 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

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Electrosynthesis of the Nylon-6 Precursor from Nitrate and Cyclohexanone over a Rutile TiO2 Catalyst

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CCS Chemistry 2025年第1期7卷 266-278页

作者： Lan Luo Lingxiu Li Liang Xu Yifan Yan Shanshan Zhang Hua Zhou Zhenhua Li Mingfei Shao Xue Duan State Key Laboratory of Chemical Resource Engineering College of ChemistryBeijing University of Chemical TechnologyBeijing 100029 College of Chemical Engineering Beijing University of Chemical TechnologyBeijing 100029 Quzhou Institute for Innovation in Resource Chemical Engineering Quzhou 324000

Electrocatalytic reduction of nitrate(NO3−)to valuable organonitrogen compounds beyond ammonia is a promising strategy for mitigating the humancaused unbalance of the global nitrogen ***,we present an electrochemical strategy for synthesizing cyclohexanone oxime(CHO),an important feedstock in nylon-6 production through hydrogenative coupling of NO_(3)^(−)and cyclohexanone(CYC)using a rutile titanium dioxide(R-TiO_(2))catalyst under ambient *** CHO productivity achieved 127.3μmol cm^(−2) h^(−1) with a high Faradaic efficiency(FE)of 68.2%at a current density of 30 mA cm^(−2).Moreover,the yield of CHO reached 98.2%.We demonstrated that the electrosynthesis of CHO operated through a tandem reaction mechanism involving the in situ generation of hydroxylamine(NH2OH)from NO_(3)^(−) reduction,followed by a spontaneous nucleophilic addition–elimination reaction between NH2OH and ***,we revealed that R-TiO_(2) exhibited a superior scaling relation with a high NH2OH generation rate and excellent CYC adsorption ability,which promoted CHO *** electrochemical strategy was also effective for the synthesis of different ***,we designed a coupling reaction system to realize the simultaneous production of CHO and CYC by combining cathodic NO3−reduction and anodic cyclohexane oxidation,demonstrating a greener and more economical approach.

关键词： electrosynthesis nitrate reduction hydroxylamine cyclohexanone oxime rutile titanium dioxide

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