CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Liqun Xia,Yi Chen,Haiyang Wu,Mingchao Wang,Gonghui Li
Reaction engineering is key to enhance enzyme-catalyzed reactions. While previous studies have focused on boosting enzyme activity, they often overlook enzyme kinetics—especially the K m ( S 0.5 ) value—that are crucial for optimal performance under physiological conditions. Herein, we developed a novel enzyme-kinetics-guided reaction engineering strategy to improve the substrate affinity of therapeutic enzymes. In this proof-of-concept experiment, we selected arginine deiminase (ADI), a promising therapeutic enzyme for treating arginine-auxotrophic tumors. First, a kinetic trap was identified, and an enzyme-kinetics-based screening model was developed to overcome it. Next, we identified and characterized a novel arginine deiminase (ADI) from Gammaproteobacteria ( Gam ADI), which was subsequently engineered to enhance its catalytic efficiency under the guidance of the kinetic model. Through ultra-high-throughput screening, two ADI variants with low S 0.5 values were identified. After recombination, the final variant GamADI M7 exhibited a remarkable improvement in substrate affinity (91 % reduction in S 0.5 value) and a 1382-fold enhancement in catalytic efficiency. The therapeutic potential of GamADI M7 was validated via cytotoxicity assays in melanoma and prostate cancer cell lines, where its IC 50 values decreased dramatically compared to wild-type ADI. This study highlights the power of enzyme-kinetics-guided reaction engineering, offering a promising strategy to enhance enzyme substrate affinity.
研究领域:
生物化学
·
分子生物学
·
肿瘤学
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产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Xing Wei,Qingqiang Wang,Xunli Zhang,Ying Chen,Nan Jin,Yuchao Zhao
The process of converting glucose into formic acid (FA) has been explored as a promising route for using biomass as a renewable feedstock for green chemical manufacturing. However, the most commonly used batch-tank reactor systems currently suffer from several drawbacks, including extended processing time, limited product selectivity, and high energy consumption, while the underlying reaction paths have been poorly understood. In this work, a continuous flow microchannel reactor was employed for the glucose conversion catalyzed by H 5 PV 2 Mo 10 O 40 with O 2 as an oxidant. The influence of various parameters on the conversion rate of glucose and the FA yield was characterized. Experimental results indicated that with a residence time of less than 3 min, the glucose was completely converted, and the highest FA yield reached 82.40 %. Extensive examination on the apparent by-products revealed that most of them acted as intermediates to produce FA through various pathways, including glyoxal, glyceraldehyde and glycolaldehyde as key intermediates for the oxidation of glucose to FA. Furthermore, the density functional theory (DFT) method was used to determine the bond energies of different C–C bond cleavage modes of substrate glucose and fructose produced by the isomerization of glucose. Experimentally, the conversion of three main intermediates and some other possible intermediates and their FA yield were measured with different residence time. It was also found that the CO 2 was produced through the decarboxylation of α-hydroxy and α-carbonyl carboxylic acid compounds, while the aldehyde groups in the compounds were more likely converted to FA by the α-carbon bond cleavage. Finally, plausible reaction pathways were proposed for the process of glucose-to-FA catalyzed by HPA-2, providing useful guidance for the identification of side reaction pathways and further improvement of FA yield.
研究领域:
化学工程
·
绿色化学
·
催化
·
反应工程
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产品关联
DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Zhixu Gan,Nikita Dewangan,Zhigang Wang,Shaomin Liu,Xiaoyao Tan,Sibudjing Kawi
The synthesis of SAPO-34 hollow fiber membranes employs the ball-milling assistant method to enhance membrane yield and quality. These membranes are then combined with CrO x /Al 2 O 3 catalyst to create a packed bed membrane reactor (PBMR) for propane dehydrogenation (PDH). The study investigates the impact of operating temperatures, weight hourly space velocities (WHSV), and sweep gas flow rates on the SAPO-34 zeolite membrane reactor's performance, comparing it to a traditional packed bed reactor (PBR). The removal of hydrogen from the reaction side significantly improves propane conversion, surpassing thermodynamic equilibrium. In PBMR, propylene selectivity slightly exceeds that in PBR, influenced by side reactions like hydrogenolysis and cracking after hydrogen removal. Furthermore, the SAPO-34 zeolite membrane reactor undergoes a prolonged stability test with frequent regeneration using pure propane as feedstock to simulate industrial conditions. It exhibits consistent performance over 120 regeneration cycles within 240 h, maintaining similar H 2 permeability and H 2 /C 3 H 8 selectivity as the fresh membrane post long-term testing.
研究领域:
化学工程
·
材料科学
·
催化
·
膜技术
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反应工程
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产品关联
DOI
高影响因子
ENERGY CONVERSION AND MANAGEMENT
·
2025
·
IF 10.9
Mingyu Liu,Sheng Chen,Jianhong Fu,Yunhao Huang,Shuang Liu,Wenqiang Liu
Thermochemical energy storage via the calcium-looping process is a highly promising technology for next-generation concentrated solar power systems. However, the development of efficient and stably operated solar-driven chemical reactors remains a significant challenge. This study provides a comprehensive investigation into the energy storage performance of Al/Fe/Mn co-doped CaCO 3 particles in a kilogram-scale, directly irradiated fluidized-bed reactor, systematically evaluating the spatiotemporal temperature distribution, reaction kinetics, and particle degradation mechanisms under varying fluidizing gas velocities. At low flow rates, a fixed-bed state resulted in severe particle sintering and incomplete reaction. Conversely, under fluidized conditions, particle conversion consistently exceeded 90%. However, while excessively high gas velocities further improved temperature uniformity, the associated convective heat loss limited the reaction rate, leading to a substantial increase in the characteristic reaction time. An optimal flow rate of 18 L/min minimized the calcination time to 18.35 min and yielded a peak solar-to-chemical energy conversion efficiency. Particle degradation was found to be governed by a complex interplay between thermal stress-induced fragmentation (dominant at low flow rates) and mechanical attrition (dominant at high flow rates). Furthermore, significant density-induced particle segregation was observed across all flow rates, with denser, unreacted CaCO 3 particles accumulating at the bottom of the bed. This study provides critical insights into the intricate trade-offs between thermal performance, material integrity, and particle dynamics, which are paramount for the rational design and reliable scale-up of solar thermochemical reactors.
研究领域:
能源材料
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化学工程
·
太阳能利用
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反应工程
·
材料科学
·
热力学
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产品关联
DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2025
·
IF 2.8
Xianhua Huan,Hong Zang,Zhiwen Ji,Siheng Liu,Chao Gao,Fusheng Zhou,Jiahe Yu,Qiulin Chen,Bin Du,Yushun Zhao
Long-chain epoxy resins are increasingly adopted in high-voltage insulation systems due to their low curing exotherm, improved toughness, and superior dielectric properties. These resins are typically synthesized via chain extension between bisphenol A and short-chain epoxy precursors. However, during pilot-scale production, inadequate heat dissipation often leads to thermal overshoot, inducing undesirable side reactions and structural irregularities. In this study, we investigate how reaction-induced thermal fluctuations affect the molecular architecture of chain-extended epoxy resins and, consequently, the performance of their cured insulation materials. Differential scanning calorimetry (DSC) and gel permeation chromatography (GPC) analyses reveal that thermal overshoots exceeding 20°C promote side reactions between hydroxyl and epoxy groups, resulting in increased molecular branching, higher viscosity, and compromised processability. These structural changes further lead to reduced crosslinking uniformity, manifested by lower crosslink density, diminished mechanical toughness (impact strength decreased from 26.4 to 24.1 kJ/m 2 ), and deteriorated dielectric performance (volume resistivity dropped from 2.58 × 10 17 to 1.94 × 10 17 Ω ·cm). This work provides mechanistic insight into the interplay between reaction conditions and structure–property evolution, offering practical guidance for the controlled and scalable production of high-performance epoxy insulation materials.
研究领域:
高分子化学
·
电气工程材料
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介电材料科学
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反应工程
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绝缘技术
·
材料结构与性能
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Lian Duan,Weiyao Yang,Hongda Zhang,Mengmeng Huang,Le Sang,Jisong Zhang
In this work, high-efficiency and continuous production of tetrahydrofurfuryl alcohol (THFA) over a Ru/C catalyst was performed in micropacked bed reactors (μPBRs). The excellent reaction performance demonstrated by the combination of μPBRs and the Ru/C catalyst resulted in a 100% furfural (FUR) conversion and a 98.5% yield of THFA within 3.5 min at 25 °C. Subsequently, a kinetic model was developed to describe the continuous hydrogenation of FUR in μPBRs. Utilizing the established kinetic model, the concentrations of various substances were predicted at different residence times between 25 and 45 °C, with an error of less than ±25%. The apparent activation energies for the FUR conversion to furfuryl alcohol (FA) and for the subsequent hydrogenation of FA to THFA were found to be 18.9 and 30.6 kJ/mol, respectively. Furthermore, the space-time yield (STY) of the μPBR system reached 0.21 kgTHFA L–1 h–1, significantly surpassing stirred tank reactors (STRs). These results demonstrate the superior efficiency and productivity of the μPBR system, providing a scalable and sustainable solution for the THFA synthesis.
研究领域:
化学工程
·
催化
·
反应工程
·
绿色化学
·
过程强化
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产品关联
DOI
高影响因子
Advanced Manufacturing-Polymer & Composites Science
·
2025
·
IF 2.2
Yating Ma,Tao Luo,Kazushi Yamada,Tingting Luo,Kunkun Fu,Xiaoyu Cui,Linmei Zhang
Frontal polymerization (FP) offers an efficient and energy-saving alternative to conventional curing methods for epoxy resins. In this study, a transient thermo-chemical coupled heat-transfer model (V-model) was developed using temperature-dependent thermophysical properties. Curing kinetics parameters were first determined by fitting data from non-isothermal differential scanning calorimetry of a BADGE-based resin. Compared to a constant-property model, accounting for changes in thermal conductivity and specific heat capacity significantly improved the accuracy of the predicted temperature profiles, aligning more closely with experimental observations. The validated V-model was then extended to evaluate the impact of boundary materials with different thermal conductivities on FP behavior. Experiments confirmed that high-conductivity boundaries facilitate preheating of unreacted resin, thereby promoting faster polymerization-wave propagation. Meanwhile, insulating boundary materials minimize heat loss, sustaining the FP reaction. This combined computational–experimental approach provides deeper insights into the heat-transfer mechanisms governing epoxy resin FP and guidance for optimizing industrial process parameters.
研究领域:
高分子材料科学
·
反应工程
·
热传导分析
·
计算材料学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Zifei Yan,Grace Dai Zhen Lee,Jian Deng,Guangsheng Luo
Nitrosation of alcohols with nitrous acid is widely used to prepare alkyl nitrites, but the reaction mechanism and formation pathways of gaseous side products remain unclear. Here, we propose a nitrosation mechanism based on a highly reactive intermediate, dinitrogen trioxide (N 2 O 3 ). The N 2 O 3 -based mechanism shows a lower energy barrier than the previously reported acid-catalyzed and nitrosyl cation mechanism. Furthermore, a microfluidic platform was established to investigate the gas–liquid-liquid reaction system and characterize the gas holdup of the multiphase reaction system. The results suggest that the reaction rate and selectivity primarily depend on the interfacial mass transfer of N 2 O 3 between the aqueous-organic and gaseous-organic phases. A tubular microreactor was employed to intensify the nitrosation process of isopropanol. In contrast to the batch process operated by adding reactants dropwise in several hours, the product yield of 95 % can be achieved in a residence time of only 10 s in the microflow reactor.
研究领域:
化学工程
·
反应工程
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产品关联
DOI
高影响因子
Sustainability
·
2024
·Vol. 16
·期 19
·8568
·
IF 3.3
Yuan-Yuan Wang,Dan-Feng Zhang,Hong-Rui Zhang,Wen-Jun Liu,Zhi-Quan Chen,Jun-Cheng Jiang,Lei Ni
In this study, sodium dodecylbenzene sulfonate was used as a stabilizer, and NaOH, TBHP, and benzoyl chloride were used as reactants in the preparation of tert–butyl peroxybenzoate (TBPB) using a two–step process. The process conditions were optimized by a three–factor, three–level Box–Behnken design approach. The results showed that the yield of TBPB achieved 88.93% under the optimum conditions of temperature of 31.50 °C, feeding time of 22.00 min, and NaOH concentration of 15%. The exothermic properties of the synthesis of TBPB were investigated using reaction calorimetry. The thermal decomposition characteristics of reactants and products were analyzed by differential scanning calorimetry (DSC) and accelerating rate calorimetry (ARC), and the changes in substance types, characteristic peaks, and exothermic quantities during the reaction were analyzed before and after the reaction by FTIR. The reaction mechanism was proposed by combining EasyMax 102, RC1e, gas chromatography (GC), and Fourier transform infrared spectrometry (FTIR). A comprehensive study of the reaction mechanism and reaction exotherm was carried out using density functional theory (DFT) to predict the reaction energy change and the direction of the reaction and to determine whether the reaction was reversible or not. The risk level for the synthesis of TBPB in semi–batch mode was evaluated using a risk matrix and the Stoessel criticality diagram. The optimal conditions for the TBPB synthesis process in a plate microreactor were explored. Both microreactors and semi–batch modes were comparatively analyzed using the m–ITHI quantitative assessment method. The results indicated a hazard class 2 in semi–batch mode and a hazard class 1 in the microreactor. The results of the study may provide a reference for the further improvement of the intrinsically safe design of the synthetic TBPB process.
研究领域:
化学工程
·
过程安全
·
热分析
·
反应工程
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产品关联
DOI
高影响因子
Nanoscale
·
2025
·
IF 5.1
Haoran Shi,Xiaotao Yang,Xinxin Cui,Hongyan Xiao,Shuai Pang,Xiang Li,Yue Long,Xiqi Zhang,Kai Song,Lei Jiang
Inspired by natural enzymes, the fabricated two-dimensional graphene oxide-based membrane reactors offer promising nanoconfined catalytic ability and mass transfer efficiency. Interestingly, for the ring-opening reaction of styrene oxide with aniline as the model reaction, abrupt modulation of nanoconfined catalytic behaviors was found by introducing binary solvents into the membrane reactors. In detail, in a binary solvent composed of ethanol and another solvent, the conversion dropped abruptly from ≈100% to less than 1% with a very small decrease in ethanol content in a certain range. Synergistic coordination of multiple physicochemical factors was explored to explain this novel modulation of nanoconfined catalytic behaviors.
研究领域:
纳米催化
·
材料化学
·
膜科学
·
绿色化学
·
反应工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2025
·
IF 3.7
Guangshuo Wu,Ziqi Cai,Zhipeng Li,Junhao Wang,Zhengming Gao
To enhance the micromixing in chemical processes, a jet-stirred tank reactor (JSTR) was developed by integrating an annular jet with the width of 0.38 mm and 0.60 mm into a 81 L stirred tank to provide localized energy intensification. The iodide–iodate reaction method was used to evaluate the micromixing performance under different operating and structural conditions. Results showed that the micromixing time determined by the incorporation model decreased with increasing impeller speed and jet width, while the feeding position and jet velocity can significantly influence the micromixing due to jet deflection. The micromixing time in the JSTR ranged from 10 to 30 ms, representing a reduction of up to 3.45 times compared with the situation that only stirred tank was used. Numerical simulations of flow in the JSTR revealed four typical flow patterns illustrating the way by which the jet can affect the micromixing within the reactor. Furthermore, an operating diagram for mapping the micromixing time based on energy dissipation rate analysis was developed.
研究领域:
化学工程
·
反应工程
·
流体动力学
·
过程强化
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2025
·
IF 3.7
Yi-Fan Xue,Fei Zhao,Jie Feng,Wen-Ying Li
In hydrofining processes, the competitive interactions among sulfur-containing compounds, aromatic hydrocarbons, and nitrogen-containing intermediates fundamentally govern catalytic performance. Nevertheless, the complex kinetic relationships within hydrodenitrogenation (HDN) systems have remained unclear and insufficiently investigated. This research comprehensively and systematically examined the competitive reaction kinetics of naphthalene (an aromatic model) and dibenzothiophene (a sulfur-based model) during the HDN of 1,2,3,4 - tetrahydroquinoline over Pt-based catalysts. Through systematic analysis of conversion rates and product distributions across various reaction conditions, it demonstrated that both dibenzothiophene and naphthalene exert distinct inhibitory effects on HDN through mechanistically differentiated pathways. Quantitative evaluation revealed a pronounced temperature dependence in mitigating these inhibitory effects, whereas pressure variations exhibited negligible influence. These findings collectively demonstrate that surface adsorption competition, rather than hydrogen availability, dictates the reaction kinetics. Rigorous kinetic calculations and rate constant fittings identified the hydrogenation of 1,2,3,4-tetrahydroquinoline to decahydroquinoline as the rate-limiting step susceptible to competitive inhibition. This phenomenon predominantly arises from the tripartite competitive adsorption among naphthalene, dibenzothiophene, and 1,2,3,4-tetrahydroquinoline at catalytic active sites, as corroborated by theoretical adsorption energy calculations. Notably, the two inhibitors manifest divergent interaction mechanisms: H + ions generated during H 2 S formation in dibenzothiophene desulfurization facilitate C–N bond cleavage, whereas naphthalene directly suppresses this critical step. Furthermore, atomic-layer-deposited TiO 2 on Pt/Al 2 O 3 engineered the catalyst surface through three synergistic effects: enhanced nitrogen adsorption capacity, optimized hydrogen spillover pathways, and generation of additional C–N bond cleavage sites. This multi-effect strategy effectively reduces the negative impacts of competitive adsorption, emphasizing the crucial role of competitive reaction kinetics in designing sulfur/aromatic-resistant HDN catalysts.
研究领域:
催化化学
·
石油炼制
·
反应工程
·
表面化学
·
材料科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）