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学者姓名：叶长燊
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Abstract ：
Ethyl methyl carbonate (EMC) serves as a vital raw material in the production of electrolytes for lithium-ion batteries. In recent years, there has been increasing focus on the development of economically efficient methods to prepare EMC through the transesterification occurring between dimethyl carbonate (DMC) and diethyl carbonate (DEC). Nevertheless, the acidic or alkaline catalysts commonly used at present are not suitable for this system. Herein, the acid-base double active site catalyst, known as [DBU+][IM−]@UiO-66, is designed and prepared to enable its application in the synthesis of EMC. The synthesis of [DBU+][IM−]@UiO-66 involves the incorporation of 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU) and imidazole (IM) molecules within the porous framework of UiO-66. The integration of these components creates an active catalyst with acid sites provided by the defect of UiO-66 and base sites derived from [DBU+][IM−] ionic liquid. The porous structure of UiO-66 offers an extensive surface area, ensuring sufficient exposure of the active sites for catalytic reactions. This catalyst combines the mutually reinforcing effects of acid and base sites, enhancing its catalytic performance and selectivity in the desired reaction. In the targeted synthesis of EMC, the [DBU+][IM−]@UiO-66 catalyst demonstrates remarkable efficiency. An EMC yield of 62% and an EMC selectivity of 99.5% were achieved, which demonstrated the effectiveness of the reaction system. The acid sites facilitate the activation of the reactants, while the base sites contribute to the formation of intermediate species. This dual functionality enhances the reaction kinetics and promotes the desired conversion of starting materials into EMC. © 2025 Institute of Process Engineering, Chinese Academy of Sciences.
Keyword ：
Acid-base bifunctional catalyst Acid-base bifunctional catalyst Ethyl methyl carbonate Ethyl methyl carbonate Ionic liquid Ionic liquid Synergistic catalyst Synergistic catalyst UiO-66 UiO-66
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| GB/T 7714 | Ge, X. , Xu, X. , Li, S. et al. Transesterification of dimethyl carbonate and diethyl carbonate over [DBU+][IM−]@UiO-66: synergistic catalysis of acid-base active sites [J]. | Green Chemical Engineering , 2025 . |
| MLA | Ge, X. et al. "Transesterification of dimethyl carbonate and diethyl carbonate over [DBU+][IM−]@UiO-66: synergistic catalysis of acid-base active sites" . | Green Chemical Engineering (2025) . |
| APA | Ge, X. , Xu, X. , Li, S. , Ye, C. , Qian, J. , Wu, Y. et al. Transesterification of dimethyl carbonate and diethyl carbonate over [DBU+][IM−]@UiO-66: synergistic catalysis of acid-base active sites . | Green Chemical Engineering , 2025 . |
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Dimethyl carbonate (DMC) is an important chemical raw material extensively used in organic synthesis, lithium-ion battery electrolytes, etc. The primary method for industrial synthesis of DMC involves transesterification between ethylene carbonate and MeOH but faces issues with difficult catalyst separation and low catalytic activity. Based on the synergistic catalytic activity of cation and anion, this study develops poly(ionic liquid)s of [NXPIL][PHO] and [N3PIL][Y] with varying alkaline sites and alkalinity levels. This is accomplished by constructing functional polymer monomers containing free radical polymerization sites and nitrogen-containing alkaline groups, and by polymerizing them with suitable cross-linking monomers in a specific ratio before exchanging the resulting polymers with different anions. Results show that doping with nitrogen-containing alkaline groups leads to enhanced basic functional sites while appropriate anions provide intensified alkalinity levels. The [N3PIL][PHO] obtained exhibits superior catalytic activity in transesterification synthesis of DMC, with a yield of 91.43% and selectivity of 99.96% at a reaction time of 2 h. The study also investigates the impact of poly(ionic liquid) cationic structure and anion types, as well as their interactions, on catalytic performance. The findings reveal that the catalytic activity of poly(ionic liquid) is restricted by the interactions between cation and anion. Based on these findings, a possible reaction mechanism was proposed, providing theoretical support for the high-efficiency production of DMC.
Keyword ：
anion and cation regulation anion and cation regulation dimethyl carbonate production dimethyl carbonate production mechanism mechanism poly(ionic liquid)s poly(ionic liquid)s transesterification reaction transesterification reaction
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| GB/T 7714 | Qi, Zhaoyang , Zhang, Fuying , Su, Huiyun et al. Functional poly(ionic liquid) with unique zwitterionic structure as efficient catalyst for the conversion of ethylene carbonate to dimethyl carbonate [J]. | SMART MOLECULES , 2025 . |
| MLA | Qi, Zhaoyang et al. "Functional poly(ionic liquid) with unique zwitterionic structure as efficient catalyst for the conversion of ethylene carbonate to dimethyl carbonate" . | SMART MOLECULES (2025) . |
| APA | Qi, Zhaoyang , Zhang, Fuying , Su, Huiyun , Ye, Changshen , Wang, Qinglian , Qiu, Ting et al. Functional poly(ionic liquid) with unique zwitterionic structure as efficient catalyst for the conversion of ethylene carbonate to dimethyl carbonate . | SMART MOLECULES , 2025 . |
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Designing efficient adsorbents for the deep removal of refractory dibenzothiophene (DBT) from fuel oil is vital for addressing environmental issues such as acid rain. Herein, zinc gluconate and urea-derived porous carbons SF-ZnNC-T (T represents the carbonization temperature) were synthesized without solvents. Through a temperature-controlled process of 'melting the zinc gluconate and urea mixture, forming H-bonded polymers, and carbonizing the polymers,' the optimal carbon, SF-ZnNC-900, was obtained with a large surface area (2280 m2 g−1), highly dispersed Zn sites, and hierarchical pore structures. Consequently, SF-ZnNC-900 demonstrated significantly higher DBT adsorption capacity of 43.2 mg S g−1, compared to just 4.3 mg S g−1 for the precursor. It also demonstrated good reusability, fast adsorption rate, and the ability for ultra-deep desulfurization. The superior DBT adsorption performance resulted from the evaporation of residual zinc species, which generated abundant mesopores that facilitated DBT transformation, as well as the formation of Zn-Nx sites that strengthened the host-guest interaction (ΔE = −1.466 eV). The solvent-free synthesized highly dispersed Zn-doped carbon shows great potential for producing sulfur-free fuel oil and for designing metal-loaded carbon adsorbents. © 2024 Institute of Process Engineering, Chinese Academy of Sciences
Keyword ：
Carbonization Carbonization Desulfurization Desulfurization Elastomers Elastomers Fuel oils Fuel oils Mesopores Mesopores
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| GB/T 7714 | Lu, Ping , Sun, Zhenhua , Ke, Xinrong et al. Solvent-free synthesis of highly dispersed zinc-doped porous carbons as efficient dibenzothiophene adsorbents [J]. | Green Energy and Environment , 2025 , 10 (5) : 994-1001 . |
| MLA | Lu, Ping et al. "Solvent-free synthesis of highly dispersed zinc-doped porous carbons as efficient dibenzothiophene adsorbents" . | Green Energy and Environment 10 . 5 (2025) : 994-1001 . |
| APA | Lu, Ping , Sun, Zhenhua , Ke, Xinrong , Ye, Changshen , Huang, Zhixian , Qiu, Ting . Solvent-free synthesis of highly dispersed zinc-doped porous carbons as efficient dibenzothiophene adsorbents . | Green Energy and Environment , 2025 , 10 (5) , 994-1001 . |
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Conjugated micro-mesoporous poly(aniline)s (CMPAs) synthesized through Buchwald-Hartwig coupling represent a cutting-edge material platform for selective sequestration of Hg (II) but suffer from moderate porosities and constrained availability of adsorption sites. Herein, we show a salt strategy for fine-tuning the porosity and Hg (II) adsorption performance of a series of S, N dual heteroatom functionalized CMPAs (CMPA-SN). The salt of NaF with appropriate dosage results in strikingly improved surface areas from 26 to 735 m2/g and intensified Hg (II) adsorption capacity from 311 mg/g to 649 mg/g. Moreover, CMPA-SN exhibits an efficient adsorption rate (h = 1250 mg/g/min) and excellent affinity with high Kd as high as 1.24 x 106 mL/g. We successfully correlate the adsorption capacity and surface area, and reveal the synergistic electron-sharing mechanism from N-containing ligands and in-situ decorated S heteroatoms, with 67.6 %/32.4 % contributions and Delta Eads = -0.419 eV/Delta Eads = -0.487 eV adsorption energy.
Keyword ：
Hansen solubility parameter Hansen solubility parameter Hg (II) adsorption Hg (II) adsorption Polymer Polymer Salt Salt Surface area Surface area
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| GB/T 7714 | Chen, Jie , Zeng, Wen , Huang, Huiyao et al. Tunable porosity and Hg (II) adsorption performance in dual heteroatom functionalized conjugated micro-mesoporous poly(aniline)s [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 363 . |
| MLA | Chen, Jie et al. "Tunable porosity and Hg (II) adsorption performance in dual heteroatom functionalized conjugated micro-mesoporous poly(aniline)s" . | SEPARATION AND PURIFICATION TECHNOLOGY 363 (2025) . |
| APA | Chen, Jie , Zeng, Wen , Huang, Huiyao , Lou, Xiaoyu , Chen, Song , Ye, Changshen et al. Tunable porosity and Hg (II) adsorption performance in dual heteroatom functionalized conjugated micro-mesoporous poly(aniline)s . | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 363 . |
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Ethyl methyl carbonate (EMC) is the most extensively used solvent in lithium-ion battery electrolytes. In recent years, the technology for producing EMC through the highly atom-economical transesterification of dimethyl carbonate and diethyl carbonate has garnered widespread attention. However, the commonly used sodium alkoxide basic catalysts exhibit poor catalytic activity due to their insolubility in this nonpolar reaction system. To address this, basic ionic liquids were confined and supported on a lipophilic carrier (UiO-66-NDC) by controlling the lipophilicity, ionic liquid loading, and pore structure through substituent groups on UiO-66-NDC. This led to the development of a catalyst with superior catalytic performance, [DBU+][IM-]@UiO-66-NDC(50). At 108.7 degrees C, a catalyst dosage of 9.7 wt %, and a 1.4:1 DMC:DEC ratio for 4 h, the yield of EMC reached 62.5%, achieving high catalytic activity for the transesterification synthesis of EMC. Furthermore, the study explored the lipophilicity variations during the modification of [DBU+][IM-]@UiO-66-NDC(X) with naphthyl groups, revealing the mechanism behind the formation of lipophilicity. Finally, using the prepared [DBU+][IM-]@UiO-66-NDC(50) catalytic material, the reaction kinetics for the transesterification synthesis of EMC from dimethyl carbonate and diethyl carbonate was investigated, providing support for the development of lithium-ion battery energy storage technology.
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| GB/T 7714 | Qi, Zhaoyang , Yan, Ruida , Luo, Xiaoyuan et al. Regulating the Lipophilicity of an Acid-Base Bifunctional Catalyst to Enhance the Performance of Catalytic Synthesis of Ethyl Methyl Carbonate [J]. | LANGMUIR , 2025 , 41 (35) : 23945-23955 . |
| MLA | Qi, Zhaoyang et al. "Regulating the Lipophilicity of an Acid-Base Bifunctional Catalyst to Enhance the Performance of Catalytic Synthesis of Ethyl Methyl Carbonate" . | LANGMUIR 41 . 35 (2025) : 23945-23955 . |
| APA | Qi, Zhaoyang , Yan, Ruida , Luo, Xiaoyuan , Li, Songyu , Qiu, Ting , Ye, Changshen . Regulating the Lipophilicity of an Acid-Base Bifunctional Catalyst to Enhance the Performance of Catalytic Synthesis of Ethyl Methyl Carbonate . | LANGMUIR , 2025 , 41 (35) , 23945-23955 . |
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The semiconductor manufacturing industry imposes stringent requirements on the metal ion content of photoresist resin monomers. Tris(2-carboxyethyl) isocyanurate (H3tci), a critical raw material for photoresist resin monomers, inevitably incorporates metal ions during production. However, its inherent carboxyethyl groups form stable coordination complexes with Cr(iii), hindering the semiconductor-grade resin monomer production. To achieve the ultra-deep removal of Cr(iii) at ultra-trace concentrations, inspired by the hard-soft-acid-base theory, we systematically modulated the electron-rich sulfonic acid group on polymers via controlled sulfonation conditions to achieve a novel series of adsorption materials (St) with ultra-high Cr(iii) adsorption affinity. The adsorption-recrystallization process using 6 g of St-V-15 could reduce the Cr(iii) concentration in a solution containing 1 g of H3tci from 840 ppb to 27.5 ppb. Furthermore, St-V-15 exhibited a maximum adsorption capacity of 145 mg g-1 calculated using the Langmuir model and a rapid initial adsorption rate of 82.92 mg g-1 min-1 at 333 K. Additionally, St-V-15 demonstrated exceptional selectivity for Cr(iii) over competing ions (e.g., K(i), Mg(ii), Na(i) and Zn(ii)) and maintained stable performance over at least 10 adsorption-desorption cycles. The superior performance originated from the chelation between Cr(iii) and the sites of O atoms (S-O and S 00000000 00000000 00000000 00000000 11111111 00000000 11111111 00000000 00000000 00000000 O) combined with the electrostatic interaction between deprotonated sulfonic acid groups and Cr(iii). These results position St-V-15 as a promising adsorption material for ultra-trace Cr(iii) removal in H3tci, offering a cost-effective solution for semiconductor-grade resin monomer production for the very first time.Keywords: Tris(2-carboxyethyl) isocyanurate; Complexed Cr(iii); Ultra-trace; Cr(iii) removal; Sulfonated polymers.
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| GB/T 7714 | Huang, Huiyao , Zhong, Shiquan , Chen, Yawen et al. Engineering sulfonated polymers for the removal of ultra-trace complexed Cr(iii) in tris(2-carboxyethyl) isocyanurate photoresist resin monomers [J]. | INDUSTRIAL CHEMISTRY & MATERIALS , 2025 , 3 (5) . |
| MLA | Huang, Huiyao et al. "Engineering sulfonated polymers for the removal of ultra-trace complexed Cr(iii) in tris(2-carboxyethyl) isocyanurate photoresist resin monomers" . | INDUSTRIAL CHEMISTRY & MATERIALS 3 . 5 (2025) . |
| APA | Huang, Huiyao , Zhong, Shiquan , Chen, Yawen , Gong, Wangquan , Ye, Changshen , Qiu, Ting et al. Engineering sulfonated polymers for the removal of ultra-trace complexed Cr(iii) in tris(2-carboxyethyl) isocyanurate photoresist resin monomers . | INDUSTRIAL CHEMISTRY & MATERIALS , 2025 , 3 (5) . |
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Tar residue produced in the phosgenation process is one of the important hazardous wastes in the toluene diisocyanate (TDI) industry. The efficient degradation and utilization of TDI tar residue have become a tough challenge for TDI enterprises worldwide. Traditional landfill and incinerator processes do not properly use the organic resources in tar residue, and they also pose a danger of soil and air contamination. This study explores aminolysis using polyamines as a highly efficient alternative to TDI tar residue valorization. Aminolysis offers high degradation rates and TDA yields without requiring added catalysts or solvents, presenting a potentially atom-economical process. Using diethylenetriamine (DETA), a TDA yield of approximately 60% alongside the value-added coproduct 1-(2-aminoethyl)-2-imidazolidone (AEI) was achieved under optimized conditions. Density functional theory (DFT) calculations and experimental results support a three-step mechanism involving a sequential amine attack on urea linkages, followed by cyclization. This work demonstrates the potential of aminolysis as a cleaner and effective route for the chemical recycling of TDI tar residue.
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| GB/T 7714 | Chai, Xu , Huang, Shengxian , Huang, Zhixian et al. Aminolysis of Toluene Diisocyanate Tar Residue Based on Polyamines: Efficient Conversion and Mechanism Exploration [J]. | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH , 2025 , 64 (29) : 14319-14328 . |
| MLA | Chai, Xu et al. "Aminolysis of Toluene Diisocyanate Tar Residue Based on Polyamines: Efficient Conversion and Mechanism Exploration" . | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH 64 . 29 (2025) : 14319-14328 . |
| APA | Chai, Xu , Huang, Shengxian , Huang, Zhixian , Wu, Chongfu , Lu, Ping , Ye, Changshen et al. Aminolysis of Toluene Diisocyanate Tar Residue Based on Polyamines: Efficient Conversion and Mechanism Exploration . | INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH , 2025 , 64 (29) , 14319-14328 . |
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Developing an efficient and sustainable method for producing ethyl methyl carbonate (EMC), a key electrolyte component in lithium-ion batteries, is essential to meet the growing industrial demand and comply with green chemistry principles. Conventional homogeneous processes suffer from excessive sodium-based solid waste and energy-intensive separations, creating an urgent need for a greener alternative. Inspired by the respiratory function of biological lungs, we have rationally designed a novel series of structured flexible ionic polymer catalysts. By introducing polar substrate-sensitive flexible adsorption networks and hydrogen bond-induced selective molecular adsorption active sites, these catalysts enable selective molecular adsorption and activation targeting towards ethanol, making them highly effective and selective with excellent durability. In a mild fixed-bed continuous reaction at 248 K, the EMC yield reaches 67% with a selectivity of over 94%; under reactive distillation conditions, the ethanol conversion exceeds 99.5% with EMC selectivity remaining above 95%. They also demonstrate exceptional operational stability for >3500 h, outperforming all base-triggered transesterification catalysts such as MOF-808. Compared with conventional sodium methoxide, more importantly, our heterogeneous catalysts eliminate 475 t a(-1) of solid waste and reduce separation energy consumption and operating costs by 20%, further quantitatively addressing the mandate of Green Chemistry. This study not only establishes a high-efficiency catalytic pathway for EMC production but also provides a generalizable strategy for designing adaptive catalysts aligned with sustainable chemical manufacturing.
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| GB/T 7714 | Cui, Rongkai , Yin, Fengyue , Gong, Wangquan et al. A bioinspired heterogeneous catalyst for green and targeted transesterification of ethanol and dimethyl carbonate to ethyl methyl carbonate with high endurance [J]. | GREEN CHEMISTRY , 2025 , 27 (36) : 11167-11178 . |
| MLA | Cui, Rongkai et al. "A bioinspired heterogeneous catalyst for green and targeted transesterification of ethanol and dimethyl carbonate to ethyl methyl carbonate with high endurance" . | GREEN CHEMISTRY 27 . 36 (2025) : 11167-11178 . |
| APA | Cui, Rongkai , Yin, Fengyue , Gong, Wangquan , Yan, Ningjing , Li, Siyao , Ye, Changshen et al. A bioinspired heterogeneous catalyst for green and targeted transesterification of ethanol and dimethyl carbonate to ethyl methyl carbonate with high endurance . | GREEN CHEMISTRY , 2025 , 27 (36) , 11167-11178 . |
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Metal foam flow field shows great potential for next-generation proton exchange membrane (PEM) fuel cell of high power density due to its well-connected pore structure, high thermal and electrical conductivity. However, the complicated pore structure makes it a challenge for water management. To tackle this issue, a novel design of metal foam flow field with hierarchical pore structure was proposed. Based on lattice Boltzmann method (LBM), the structure-performance relationship between hierarchical pore structure and water discharge capability of flow field was explored by using breakthrough time. Furthermore, an optimal hierarchical pore structure for metal foam flow field that shows superior water discharge capability was obtained. Compared with metal foam with uniform coarse pore structure, breakthrough time can be reduced roughly by 17.6% in the one with optimal hierarchical pore structures. This finding provides a theoretical foundation and technical guidance for developing metal foam flow field.
Keyword ：
hierarchical pore structure hierarchical pore structure lattice Boltzmann method (LBM) lattice Boltzmann method (LBM) metal foam flow field metal foam flow field proton exchange membrane (PEM) fuel cell proton exchange membrane (PEM) fuel cell water discharge capability water discharge capability
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| GB/T 7714 | Lin, Yixiong , Sun, Yun , Yang, Chen et al. Liquid water discharge capability enhancement of hierarchical pore structure in metal foam flow field of proton exchange membrane fuel cell [J]. | AICHE JOURNAL , 2024 , 70 (1) . |
| MLA | Lin, Yixiong et al. "Liquid water discharge capability enhancement of hierarchical pore structure in metal foam flow field of proton exchange membrane fuel cell" . | AICHE JOURNAL 70 . 1 (2024) . |
| APA | Lin, Yixiong , Sun, Yun , Yang, Chen , Zhang, Wei , Wang, Qinglian , Wan, Zhongmin et al. Liquid water discharge capability enhancement of hierarchical pore structure in metal foam flow field of proton exchange membrane fuel cell . | AICHE JOURNAL , 2024 , 70 (1) . |
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Biodiesel, known as a renewable fuel, is an environmentally friendly energy source derived from animal and vegetable oils, as well as recycled oil. Despite this, the current advancements in biodiesel technology face challenges in fully replacing petrochemical diesel, primarily due to the non-green catalytic synthesis and high production cost associated with biodiesel. Ionic liquids containing strong Lewis acids or BrOnsted acids have been highlighted as a novel class of environmentally friendly solvents and catalysts, showing green and effective catalytic potential in the synthesis of biodiesel via transesterification. In another aspect, reactive distillation technology could facilitate continuous forward reactions catalyzed by ionic liquids by swiftly removing reaction products from the reaction zone, offering advantages in improving the production efficiency, energy consumption, and cost reduction. From this perspective, we discuss the synthesis of biodiesel catalyzed by ionic liquids, supported ionic liquids, amphiphilic ionic liquids, and amphiphilic supported ionic liquids. The focus is on the process for synthesizing biodiesel through catalytic distillation. We emphasize the potential role of the lipophilic group in the ionic liquid catalyst, promoting the mutual solubility of the reactant triglyceride with methanol or ethanol. This enhancement might facilitate contact between the reactants and improve the catalytic efficiency of transesterification. Additionally, we propose several methods to improve the efficiency of biodiesel synthesis catalyzed by ionic liquid catalysts and suggest appropriate reactive distillation processes for biodiesel production.
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| GB/T 7714 | Qi, Zhaoyang , Cui, Rongkai , Lin, Hao et al. Challenges and perspectives on using acidic ionic liquids for biodiesel production via reactive distillation [J]. | GREEN CHEMISTRY , 2024 , 26 (13) : 7718-7731 . |
| MLA | Qi, Zhaoyang et al. "Challenges and perspectives on using acidic ionic liquids for biodiesel production via reactive distillation" . | GREEN CHEMISTRY 26 . 13 (2024) : 7718-7731 . |
| APA | Qi, Zhaoyang , Cui, Rongkai , Lin, Hao , Ye, Changshen , Chen, Jie , Qiu, Ting . Challenges and perspectives on using acidic ionic liquids for biodiesel production via reactive distillation . | GREEN CHEMISTRY , 2024 , 26 (13) , 7718-7731 . |
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