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Energy & Environmental Materials 2024年第1期7卷 188-196页

作者： Changyu Leng Zongbin Zhao Xuzhen Wang Yuliya V.Fedoseeva Lyubov G.Bulusheva Alexander V.Okotrub Jian Xiao Jieshan Qiu State Key Lab of Fine chemicals School of Chemical Engineering Liaoning Key Lab for Energy Materials and Chemical Engineering Dalian University of Technology Nikolaev Institute of Inorganic Chemistry Siberian Branch of the Russian Academy of Sciences College of chemical engineering Beijing University of Chemical Technology

Metal-organic framework(MOF)-derived carbon composites have been considered as the promising materials for energy ***,the construction of MOF-based composites with highly controllable mode via the liquid-liquid synthesis method has a great challenge because of the simultaneous heterogeneous nucleation on substrates and the self-nucleation of individual MOF nanocrystals in the liquid phase.

关键词： carbon composite electrostatic interaction metal–organic framework coating self-assembly zinc-ion hybrid capacitor

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

Amorphous hybrid tungsten oxide–nickel hydroxide nanosheets used as a highly efficient electrocatalyst for hydrogen evolution reaction

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Nano research 2024年第4期17卷 2499-2508页

作者： Chao Lyu Chenghai Dai Yiwei Tan State Key Laboratory of Materials-Oriented chemical engineering School of Chemistry and Chemical EngineeringNanjing Tech UniversityNanjing 211816China

There are more challenges for alkaline hydrogen evolution reaction(HER)via simultaneously expediting the electron-coupled water dissociation process(Volmer step)and the following electrochemical H_(2) desorption(Heyrovsky step).Hybrid amorphous electrocatalysts are highly desirable for efficient hydrogen evolution from water-alkali electrolyzers due to the bifunctionality for the different elementary steps of HER and optimal interactions with water molecules and the reactive hydrogen intermediates(Had).Herein,the synthesis of amorphous hybrid ultrathin(tungsten oxide/nickel hydroxide)hydrate(a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O)nanosheets on nickel foam(NF)for efficient alkaline HER is *** structural and composition features of a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O are characterized in *** resulting a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O/NF electrocatalyst with the synergistic effect of both hybrid components for the HER elementary steps shows greatly improved the activity and durability for the HER with a low overpotential of-41 and-163 mV at-10 and-500 mA·cm^(-2),respectively,a Tafel slope as low as-72.9 mV·dec^(-1),and long-term stability of continuous electrolysis for at least 150 h accompanying by inappreciable overpotential change in 1 M *** the hybrid a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O,Ni(OH)_(2) and WO_(3) moieties are separately responsible for accelerating dissociative adsorption of water and weakening Had adsorption strength,which is beneficial to the improvement of the alkaline HER activity.

关键词： amorphous nanomaterial bimetallic electrocatalyst tungsten oxide ultrathin nanosheet hydrogen evolution reaction

Cobalt-based deep eutectic solvent modified nitrogen-doped carbon catalyst for boosting oxygen reduction reaction in zinc-air batteries

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Chinese Journal of Structural Chemistry 2024年第1期43卷 33-39页

作者： Peng Wang Daijie Deng Suqin Wu Li Xu Institute for Energy research School of Chemistry and Chemical EngineeringJiangsu UniversityZhenjiang212013China

As an oxygen reduction reaction(ORR)catalyst,nitrogen-doped carbon(NC)is widely used in zinc-air batteries(ZABs).However,NC catalysts exhibit low conductivity and insufficient exposure of active ***,a Co-based deep eutectic solvent(DES)was selected to modify NC catalyst(Co-NC)to improve ORR *** functional theory(DFT)calculation shows that the modification of Co-based DES can change the electronic structure of NC and increase metallic active sites,which is beneficial to the desorption of reaction intermediates on Co-NC,further improving ORR ***-NC shows excellent ORR performances and ***,ZABs assembled with Co-NC manifest a high maximum power density of 177.4 mW cm^(-2),a high specific capacity of 726.12 mA h g^(-1)and a charge-discharge cycle life of 500 *** study can provide practical reference for surface modified carbon-based electrocatalyst with DES to improve ORR performances.

关键词： Deep eutectic solvent Nitrogen-doped carbon Surface modification Oxygen reduction reaction Zinc-air battery

Insights into the role of oxygen-containing functional groups on carbon surface in water–electricity generation

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Nano research 2024年第7期17卷 6645-6653页

作者： Wan Xue Zongbin Zhao Honghui Bi Bolun Zhang Xuzhen Wang Jieshan Qiu State Key Laboratory of Fine chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China State Key Laboratory of Fine chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of ChemistryDalian University of TechnologyDalian 116024China State Key Laboratory of chemical Resource engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

A deep understanding of the electricity generation mechanism from the interaction between water molecules and carbon material surfaces is attractive for next-generation water-based energy conversion and storage ***,an asymmetric generator was assembled based on functionalized carbon nanotubes films to investigate the relative contribution from various oxygen functional groups on carbon surface to the water-electrical *** and calculations demonstrate that the electricity mainly originates from the water molecule adsorption by carboxyl groups and dissociation of functional groups on carbon surface,which leads to the formation of electrical double layers at *** device allows the electricity generation with a variety of water sources,such as deionized water,tap water,as well as *** particular,the generator based on carboxyl carbon nanotubes can induce a voltage of over 200 mV spontaneously in natural seawater with the power density of about 0.11 mW·g^(−1).High voltages can be achieved easily through the series-connection strategy to power electronic products such as a liquid crystal *** work reveals the dominant role of carboxyl groups in carbon-based water–electricity conversion and is expected to offer inspiration for the preparation of carbon materials with high electrical performance.

关键词： electricity generation water adsorption dissociation carboxyl groups carbon nanotubes

Photocatalytic activation of sulfite by N-doped porous biochar/MnFe_(2)O_(4) interface-driven catalyst for efficient degradation of tetracycline

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Green Energy & Environment 2024年第3期9卷 481-494页

作者： Long Cheng Yuanhui Ji Jiangsu Province Hi-Tech Key Laboratory for Biomedical research School of Chemistry and Chemical EngineeringSoutheast UniversityNanjing211189China

A novel photo-catalytic system composed of N-doped biochars(NBCs),MnFe_(2)O_(4) and sulfite activation under ultraviolet(NBCs/MnFe_(2)O_(4)/sulfite/UV)was constructed to realize the efficient eliminate of tetracycline(TC).As the carrier of MnFe_(2)O_(4),NBCs were synthesized from alfalfa,which has large specific surface area,graphite like structure and hierarchical porous *** adsorption isotherm indicated that NBCs/MnFe_(2)O_(4)-2:1 had the best adsorption performance for TC(347.56 mg g^(-1)).Through synergistic adsorption and photocatalysis,the removal rate of TC reached 84%,which was significantly higher than that of MnFe_(2)O_(4).Electrochemical impedance spectroscopy(EIS)and Photoluminescence(PL)characterization results showed that the introduction of NBCs improved the separation efficiency of photogenerated electron and hole pairs and enhanced the photocatalytic ***,the adsorption,degradation mechanism and degradation path of TC by the catalyst were systematically analyzed by coupling HPLC–MS measurement with the theoretical *** the advantages of excellent degradation performance,low cost,easy separation and environmental friendliness of NBCs/MnFe_(2)O_(4),this work was expected to provide a new path for the practical application of biochar.

关键词： Biochar MnFe_(2)O_(4) Sulfite Adsorption Photocatalysis

The flow behavior of droplet adsorption on a liquid-liquid interface accompanied by cross-linking reaction and phase separation in a microchannel

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Chinese Journal of chemical engineering 2024年第2期66卷 60-70页

作者： Haozhe Yi Taotao Fu Chunying Zhu Youguang Ma State Key Laboratory of chemical engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

The adsorption process of droplets on the liquid-liquid interface and phase separation process can regulate the spatial distribution of the fluid system,which are crucial for chemical ***,the cross-linking reaction,which is widely used in the field of polymers,can change the physical properties of the fluids and affect the flow behavior accordingly.A configuration of microchannels is designed to conveniently generate uniform droplets in one phase of the parallel *** flow behavior of the adsorption process of sodium alginate droplets on the liquid-liquid interface is investigated,and the subsequent process of phase separation is *** the process of droplet adsorption,the crosslinking reaction occurs synchronously,which makes the droplet viscosity and the elasticity modules of the droplet surface increase,thus affecting the dynamics of the adsorption process and the equilibrium shape of the *** variation of the adsorption length with time is divided into three stages,which all conform to power law *** exponents of the second and third stages deviate from the results of the Tanner's *** flow pattern maps of droplet adsorption and phase separation are drawn,and the operating ranges of complete adsorption and complete separation are *** study provides a theoretical basis for further studying the flow behavior of droplets with cross-linking reaction in a microchannel.

关键词： Microfluidics Droplet Dynamics Crosslink Adsorption Separation

The principle and amelioration of lithium plating in fast-charging lithium-ion batteries

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Journal of Energy Chemistry 2024年第10期97卷 453-459页

作者： Yi Yang Xia-Lin Zhong Lei Xu Zhuo-Lin Yang Chong Yan Jia-Qi Huang School of Materials Science and engineering Beijing Institute of Technology Advanced research Institute of Multidisciplinary Science Beijing Institute of Technology Beijing Key Laboratory of Green chemical Reaction engineering and Technology Department of Chemical Engineering Tsinghua University Yangtze River Delta Graduate School of Beijing Institute of Technology

Fast charging is restricted primarily by the risk of lithium（Li） plating,a side reaction that can lead to the rapid capacity decay and dendrite-induced thermal runaway of lithium-ion batteries（LIBs）.Investigation on the intrinsic mechanism and the position of Li plating is crucial to improving the fast rechargeability and safety of ***,we investigate the Li plating behavior in porous electrodes under the restricted transport of Li+.Based on the theoretical model,it can be concluded that the Li plating on the anodeseparator interface（ASI） is thermodynamically feasible and kinetically ***,the prior deposition of metal Li on the ASI rather than the anode-current collector interface（ACI） is verified *** order to facilitate the transfer of Li+among the electrode and improve the utilization of active materials without Li plating,a bilayer asymmetric anode composed of graphite and hard carbon（GH） is *** and simulation results suggest that the GH hybrid electrode homogenizes the lithiated-rate throughout the electrode and outperforms the pure graphite electrode in terms of the rate performance and inhibition of Li *** work provides new insights into the behavior of Li plating and the rational design of electrode structure.

关键词： Fast charging Graphite Hard carbon Lithium plating Lithium-ion batteries

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

Effect of solvent on the initiation mechanism of living anionic polymerization of styrene:A computational study

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Chinese Journal of chemical engineering 2024年第5期69卷 135-142页

作者： Shen Li Yin-Ning Zhou Zhong-Xin Liu Zheng-Hong Luo School of chemical engineering and Technology Hainan UniversityHaikou 570228China Department of chemical engineering School of Chemistry and Chemical EngineeringState Key Laboratory of Metal Matrix CompositesShanghai Jiao Tong UniversityShanghai 200240China

For living anionic polymerization(LAP),solvent has a great influence on both reaction mechanism and *** this work,by using the classical butyl lithium-styrene polymerization as a model system,the effect of solvent on the mechanism and kinetics of LAP was revealed through a strategy combining density functional theory(DFT)calculations and kinetic *** terms of mechanism,it is found that the stronger the solvent polarity,the more electrons transfer from initiator to solvent through detailed energy decomposition analysis of electrostatic interactions between initiator and solvent ***,we also found that the stronger the solvent polarity,the higher the monomer initiation energy barrier and the smaller the initiation rate ***,initiation is more favorable at lower temperatures based on the calculated results ofΔG_(TS).Finally,the kinetic characteristics in different solvents were further examined by kinetic *** is found that in benzene and n-pentane,the polymerization rate exhibits first-order ***,slow initiation and fast propagation were observed in tetrahydrofuran(THF)due to the slow free ion formation rate,leading to a deviation from first-order kinetics.

关键词： Living anionic polymerization Solvent effect Reaction kinetics Computational chemistry Mathematical modeling Kinetic modeling