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Journal of Energy Chemistry 2024年第10期97卷 110-119页

作者： Enduo Dai Wei An Ruixian Guo Xugen Shi Yunyi Li Yibo Wang Mingming Liu college of Chemistry and chemical engineering Shanghai University of Engineering Science

The catalytic descriptor with operational feasibility is highly desired towards rational design of high-performance catalyst especially the electrode/electrolyte solution interface working under mild ***,we demonstrate that the descriptor Ω parameterized by readily accessible intrinsic properties of metal center and coordination is highly operational and efficient in rational design of single-atom catalyst（SAC） for driving electrochemical nitrogen reduction（NRR）.Using twodimensional metal（M）-BxPySzNm@C2N as prototype SAC models,we reveal that*N2+（H++e-）→*N2H acts predominantly as the potential-limiting step（PLS） of NRR on M-B2P2S2@C2N and M-B1P1S1N3@C2N regardless of the distinction in coordination *** the 28 screened M active sites,with Ω values close to the optimal 4,M-B2P2S2@C2N(M=V（Ω=3.53）,Mo（Ω=5.12）,and W（Ω=3.92）) and M-B1P1S1N3@C2N(M=V（Ω=3.00）,Mo（Ω=4.34）,and W（Ω=3.32）) yield the lowered limiting potential（UL） as-0.45,-0.54.-0.36,-0.58,-0.25,and-0.24 V,respectively,thus making them the promising NRR *** importantly,these SACs are located around the top of volcano-shape plot of ULversus Ω,re-validating Ω as an effective descriptor for accurately predicting the high-activity NRR SACs even with complex *** study unravels the relationship between active-site structure and NRR performance via the descriptor Ω,which can be applied to other important sustainable electrocatalytic reactions involving activation of small molecules via σ-donation and π*-backdonation mechanism.

关键词： Descriptor DFT Electrocatalysis N2 reduction Single-atom catalyst

Process intensification for the synthesis and purification of battery-grade Li_(2)CO_(3)with microfluidics

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Particuology 2024年第7期90卷 106-117页

作者： Haodu Li Jie Zhang Lin Dai Le Du Jiqin Zhu The State Key Laboratory of chemical Resource engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Battery-grade lithium carbonate(Li_(2)CO_(3))with a purity of higher than 99.5 wt%is of great importance as a high value-added lithium ***,influences of different reaction systems and process control on product purity remain ***,a membrane dispersion microreactor was used to enhance the mass transfer of preparation and purification processes in homogeneous and heterogeneous *** systems of Na_(2)CO_(3)–LiCl,NH_(4)HCO_(3)–LiCl,and NH_(3)·H_(2)O−CO_(2)−LiCl,CO_(2)purification based on carbonation and decomposition were *** Li_(2)CO_(3)purity was increased by the improvement of mixing *** carbonation time was reduced by 62.5%and 58.3%for the NH_(3)·H_(2)O−CO_(2)and CO_(2)purification systems,*** the two ammonia-based systems,Li_(2)CO_(3)particles with a purity of 99.7–99.8 wt%were one-step prepared with a size of 3–5μm,which also met the requirement of the battery-grade *** purity was further increased to 99.9 wt%by CO_(2)purification and LiHCO_(3)*** investigation could provide a feasible alternative for the controllable preparation of battery-grade Li_(2)CO_(3)in one or multiple steps.

关键词： Microfluidics Battery grade Li_(2)CO_(3) Process intensification High purity

Controllable Ring-opening Polymerization ofδ-Valerolactone Catalyzed by Quinolinyl-Urea/MTBD Systems

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Chinese Journal of Polymer Science 2024年第8期42卷 1103-1110页

作者： Xin-Yu Liu Liang Zhu Su-Yun Jie Bo-Geng Li State Key Laboratory of chemical engineering College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310058China

Due to their excellent biocompatibility and biodegradability,aliphatic polyesters are widely used in the biomedical,packaging and agricultural fields,which are usually accessed by the ring-opening polymerization(ROP)of lactones and the catalysts particularly play an important *** a series of quinolinyl-urea catalysts have been synthesized via the reaction between isocyanate and aminoquinoline with an amino group at different substitution positions and *** combination with 7-methyl-1,5,7-triazabicyclo[4,4,0]dec-5-ene(MTBD)as a cocatalyst and benzyl alcohol(BnOH)as an initiator,1-(3,5-bis(trifluoromethyl)phenyl)-3-(quinolin-3-yl)urea(3-QU)was observed to be most active for the ROP ofδ-valerolactone(δ-VL).The polymerization conditions were optimized by varying the type of organic base,catalyst concentration and reaction *** changing the ratio of[M]_0/[I],linear polyvalerolactones(PVLs)with different molecular weights and narrow molecular weight distribution were *** kinetic and chain extension experiments were carried out to prove the"living"/controllable *** the NMR experiments were used to support the proposal of possible mechanism.

关键词： Quinolinyl-urea Ring-opening polymerization PVL

A thermodynamic view on the in-situ carbon dioxide reduction by biomass-derived hydrogen during calcium carbonate decomposition

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Chinese Journal of chemical engineering 2024年第4期68卷 231-240页

作者： Peng Jiang Hao Zhang Guanhan Zhao Lin Li Tuo Ji Liwen Mu Xiaohua Lu Jiahua Zhu State Key Laboratory of Materials-oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China

In the carbonate industry,deep decarbonization strategies are necessary to effectively remediate CO_(2).These strategies mainly include both sustainable energy supplies and the conversion of CO_(2)in downstream *** study developed a coupled process of biomass chemical looping H2 production and reductive calcination of CaCO_(3).Firstly,a mass and energy balance of the coupled process was established in Aspen *** this,process optimization and energy integration were implemented to provide optimized operation ***,a life cycle assessment was carried out to assess the carbon footprint of the coupled *** reveal that the decomposition temperature of CaCO_(3)in an H_(2)atmosphere can be reduced to 780℃(generally around 900℃),and the conversion of CO_(2)from CaCO_(3)decomposition reached 81.33%with an H2:CO ratio of 2.49 in gaseous *** optimizing systemic energy through heat integration,an energy efficiency of 86.30%was ***,the carbon footprint analysis revealed that the process with energy integration had a low global warming potential(GWP)of-2.624 kg·kg^(-1)(CO_(2)/CaO).Conclusively,this work performed a systematic analysis of introducing biomass-derived H_(2)into CaCO_(3)calcination and demonstrated the positive role of reductive calcination using green H_(2)in mitigating CO_(2)emissions within the carbonate industry.

关键词： Biomass CaCO_(3)reductive calcination chemical looping Hydrogen production Carbon footprint Thermodynamics process

Recent progress on nanomaterial-based electrochemical dissolved oxygen sensors

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Chinese Journal of chemical engineering 2024年第4期68卷 103-119页

作者： Shaoqi Zhang Tao Liu Zhenyu Chu Wanqin Jin State Key Laboratory of Materials-Oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China

Dissolved oxygen(DO)usually refers to the amount of oxygen dissolved in *** the environment,medicine,and fermentation industries,the DO level needs to be accurate and capable of online monitoring to guide the precise control of water quality,clinical treatment,and microbial *** with other analytical methods,the electrochemical strategy is superior in its fast response,low cost,high sensitivity,and portable ***,an electrochemical DO sensor faces a trade-off between sensitivity and long-term stability,which strongly limits its practical *** solve this problem,various advanced nanomaterials have been proposed to promote detection performance owing to their excellent electrocatalysis,conductivity,and chemical ***,in this review,we focus on the recent progress of advanced nanomaterial-based electrochemical DO *** the comparison of the working principles on the main analysis techniques toward DO,the advantages of the electrochemical method are *** is placed on recently developed nanomaterials that exhibit special characteristics,including nanostructures and preparation routes,to benefit DO ***,we also introduce some interesting research on the configuration design of the electrode and device,which is rarely ***,the different requirements of the electrochemical DO sensors in different application fields are included to provide brief guidance on the selection of appropriate ***,the main challenges are evaluated to propose future development prospects and detection strategies for nanomaterial-based electrochemical sensors.

关键词： Nanomaterial Dissolved oxygen Electrochemical sensor Nanostructures Detection principles

Towards carbon neutrality of calcium carbide-based acetylene production with sustainable biomass resources

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Green Energy & Environment 2024年第6期9卷 1068-1078页

作者： Peng Jiang Guanhan Zhao Hao Zhang Tuo Ji Liwen Mu Xiaohua Lu Jiahua Zhu State Key Laboratory of Materials-oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing211816China

Acetylene is produced from the reaction between calcium carbide(CaC_(2))and water,while the production of CaC_(2) generates significant amount of carbon dioxide not only because it is an energy-intensive process but also the raw material for CaC_(2) synthesis is from ***,a comprehensive biomass-to-acetylene process was constructed that integrated several units including biomass pyrolysis,oxygen-thermal CaC_(2) fabrication and calcium *** comparison,a coal-to-acetylene process was also established by using coal as *** carbon efficiency,energy efficiency and environmental impacts of the bio-based calcium carbide acetylene(BCCA)and coal-based calcium carbide acetylene(CCCA)processes were systematically ***,the environmental impacts were further evaluated by applying thermal integration at system level and energy substitution in CaC_(2) *** though the BCCA process showed lower carbon efficiency and energy efficiency than that of the CCCA process,life cycle assessment demonstrated the BCCA(1.873 kgCO_(2eq) kg-prod^(-1))a lower carbon footprint process which is 0.366 kgCO_(2eq) kg-prod^(-1) lower compared to the CCCA *** sustainable energy(biomass power)substitution in CaC_(2) furnace,an even lower GWP value of 1.377 kgCO_(2eq) kg-prod^(-1) can be achieved in BCCA *** work performed a systematic analysis on integrating biomass into industrial acetylene production,and revealed the positive role of biomass as raw material(carbon)and energy supplier.

关键词： Biomass pyrolysis CO_(2)mitigation Calcium carbide Acetylene Calcium loop

Preparation of PVA/GO/h-BN Janus Film with High Thermal Conductivity and Excellent Flexibility via a Density Deposition Self-assembly Method

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Chinese Journal of Polymer Science 2024年第8期42卷 1217-1226页

作者： Fang-Hua Luo Zhi-Tao Dong Guo-Hua Chen Chen Ma Huai-Yuan Wang college of Chemistry and chemical engineering Northeast Petroleum UniversityDaqing 163318China college of Materials Science and engineering Huaqiao UniversityXiamen 361000China School of chemical engineering and Technology and State Key Laboratory for chemical engineering Tianjin UniversityTianjin 300350China

Janus films with asymmetric physical/chemical properties have attracted con siderable attention due to their promising applications in personal thermal management,electronic skin s,sensors,actuators,***,traditional methods for fabricating Janus films conventionally need the assistance of an interface or auxiliary equipment,which are usually complex and ***,flexible poly(vinyl alcohol)(PVA)/graphene oxide(GO)/h-BN(recorded as PVA/GO/h-BN)Janus films with thermally,optically,and electrically anisotropic properties are fabricated by a simple density deposition self-assem bly method,which just utilizes the density difference between GO and h-BN during water *** results show that the two sides of the acquired Janus films have obvious asymmetric *** the original state of the PVA/GO/h-BN Janus films,the thermal conductivity of the GO side(10.06 W·m^(-1)·K^(-1))is generally lower than that of the h-BN side(10.48W·m^(-1)·K^(-1)).But after GO is reduced,the thermal conductivity of the rGO side reaches 12.17 W·m^(-1)·K^(-1),surpassing that of the h-BN *** addition,the relative reflectance of the h-BN side of Janus film is also significantly higher than that of the rGO side,and the su rface resistance difference between the two sides is about 4 orders of *** prepared PVA/GO/h-BN Janus films show great application potential in human thermal management,light conversion switches,and electronic *** study provides a simple and versatile strategy for fabricating Janus films with multifunctional(such as thermal,optical,and electrical)anisotropies.

关键词： Janus films PVA/GO/h-BN Density deposition self-assembly method

Catalytically generated noncovalent ammonium dienolate:a versatile platform for the development of organocatalytic asymmetric cascade reactions

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Science China Chemistry 2024年第8期67卷 2524-2546页

作者： Jun-Bing Lin Dong-Sheng Ji Peng-Fei Xu State Key Laboratory of Applied Organic Chemistry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China Shaanxi Key Laboratory of chemical Reaction engineering College of Chemistry and Chemical EngineeringYan’an UniversityYan’an 716000China

Organocatalytic cascade reactions represent a powerful strategy for the rapid construction of complex chiral molecules with multiple stereocenters from simple substrates under mild conditions. The intriguing structural feature and diverse reactivity of catalytically generated dienolate species render them competent and versatile intermediates for the development of practical and valuable cascade reactions. Over the past years, a plethora of innovative and pioneering noncovalent ammonium dienolatemediated cascade reactions have been designed and implemented under the catalysis of chiral organocatalysts, making dienolate activation a general, robust, and complementary method for the functionalization of unsaturated carbonyl compounds and related substances. This review illustrates the recent advances in organocatalytic noncovalent ammonium dienolate-mediated cascade reactions(mainly from 2010 to 2023), including the cascade transformations of ammonium dienolates directly generated from unsaturated ketone/aldehyde, ester/lactone/azlactone, amide/lactam/pyrazolone/oxindole, and alkylidene nitrile compounds. The contents are arranged based on the reaction types of the ammonium dienolates, with an emphasis on cascade 2,5-, 3,5-, and 4,5-difunctionalizations of these intermediates. Furthermore, other cascade reactions involving the 1,3-, 2,3-, and even more complex 3,4,5-reactivities of ammonium dienolates were also discussed. The reaction pathway, reaction stereoinduction, and synthetic applications of the ammonium dienolate-mediated cascade reactions were highlighted throughout the article. As a stimulating and ever-growing research area, the organocatalytic noncovalent ammonium dienolate-mediated cascade reactions are expected to continue demonstrating their magic power for constructing chiral targets in the future and further expanding the boundaries of asymmetric catalysis.

关键词： organocatalysis asymmetric catalysis ammonium dienolate cascade reaction difunctionalization

Recent advances in Pt catalysts and membrane electrode assemblies fabrication for proton exchange membrane fuel cells

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Rare Metals 2024年第9期43卷 4198-4221页

作者： Miao Ma Li-Xiao Shen Jing Liu Bin Xu Yun-Long Zhang Lei Zhao Zhen-Bo Wang School of Chemistry and chemical engineering Harbin Instituteof Technology college of Environmental and chemical engineering YanshanUniversity Unipower Hydrogen Technology (Jiangsu) Corporation

Proton exchange membrane fuel cells(PEMFCs) have been identified as a highly promising means of achieving sustainable energy conversion. A crucial factor in enhancing the performance of PEMFCs for further potential energy applications is the advancement in the field of catalyst engineering that has led to remarkable performance enhancement in facilitating the oxygen reduction reaction(ORR). Subsequently, it is important to acknowledge that the techniques used in preparation of membrane electrode assemblies(MEAs), the vital constituents of PEMFCs, also possess direct and critical influence on exhibiting the full catalytic activity of meticulously crafted catalysts. Here, a succinct summary of the most recent advancements in Pt catalysts for ORR was offered and their underly catalytic mechanism were discussed. Then, both laboratory-scale and industrial-scale MEA fabrication techniques of Pt catalysts were summarized. Furthermore, a detailed analysis of the connections between materials, process, and performance in MEA fabrication was presented in order to facilitate the development of optimal catalyst layers.

关键词： MEA fabrication techniques Membrane electrode assemblies Oxygen reduction reaction Pt catalysts

Tailoring NH4+ storage by regulating oxygen defect in ammonium vanadate

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Green Energy & Environment 2024年第7期9卷 1171-1182页

作者： Yanyan Liu Ziyi Feng Hanmei Jiang Xueying Dong Changgong Meng Yifu Zhang State Key Laboratory of Fine chemicals School of Chemical Engineering Dalian University of Technology college of Environmental and chemical engineering Dalian University

Defect engineering is an effective strategy for modifying the energy storage materials to improve their electrochemical ***, the impact of oxygen defect and its content on the electrochemical performances in the burgeoning aqueous NH+4storage field remains explored. Therefore, for the first time in this work, an oxygen-defective ammonium vanadate [（NH4）2V10O25·8H2O, denoted as Od-NHVO] with a novel 3D porous flower-like architecture was achieved via the reduction of thiourea in a mild reaction condition, which is a facile method that can realize the intention to regulate the oxygen defect content, with the capability of mass-production. The as-prepared OdM-NHVO with moderate oxygen defect content can deliver a stable specific capacitance output(505 F g-1, 252 mAh g-1at 0.5 A g-1with ～80% capacitance retention after 10,000 cycles), which benefits from extra active sites, unimpeded NH+4-migration path and relatively high structure integrity. In contrast, low oxygen defect content will lead to the torpid electrochemical reaction kinetics while too high content of it will reduce the chargestorage capability and induce structural disintegration. The superior NH+4-storage behavior is achieved with the reversible intercalation/deintercalation process of NH+4accompanied by forming/breaking of hydrogen bond. As expected, the assembled flexible OdM-NHVO//PTCDI quasi-solid-state hybrid supercapacitor（FQSS HSC） also exhibits high areal capacitance, energy density and reliable flexibility. This work provides a new avenue for developing materials with oxygen-deficient structure for application in various aqueous non-metal cation storage systems.

关键词： Ammonium vanadate Oxygen defect Ammonium-ion storage Hybrid supercapacitors Electrochemical performance