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Water-lean ionic liquid absorbents for energy-efficient CO2 capture from flue gas: Continuous experiments and techno-economic evaluation

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Chemical engineering Journal 2025年 515卷

作者： Song, Yongzheng Wang, Peng Jiang, Haiyan Li, Kaikai Zeng, Shaojuan Zhang, Xiangping Beijing Key Laboratory of Solid State Battery and Energy Storage Process CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Mesoscience and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China College of Chemical and Engineering University of Chinese Academy of Sciences Beijing100049 China College of Chemical Engineering and Environment China University of Petroleum Beijing102249 China

In this work, continuous CO2 absorption–desorption experiments under simulated flue gas (CO2, N2, O2, SO2 and NO) conditions and techno-economic analysis of CO2 capture using a novel water-lean ionic liquid (IL) absorbent (80 wt% IL, 14 wt% sulfoxide and 6 wt% water) were comprehensively combined to evaluate the feasibility of industrial applications. Thermodynamic and kinetic properties of the absorbent such as heat capacity, thermal conductivity, and absorption rate were explored and a reliable thermodynamic model was conducted. Meanwhile, continuous absorption–desorption experiments were carried out using a laboratory-scale continuous flow system (LCFS) to optimize operational parameters and assess the absorbent stability. Under optimal conditions, the CO2 concentration in the purified gas can be reduced to 0.70 mol%, and the capture efficiency was as high as 95.76 %. After 650 h of continuous experiments under simulated flue gas, the IL concentration in the absorbent remained essentially unchanged, showing excellent stability. Based on above experimental results, a process model was developed in ASPEN Plus and validated. The validated model was further scaled up to a commercial scale and a techno-economic analysis was performed to evaluate the energy consumption and cost. The regeneration energy consumption (Qreg) for the absorbent was 1.31 GJ tCO2-1, and the total cost of capture was 38.81 $ tCO2-1, indicating strong potential for industrial application. © 2025 Elsevier B.V.

关键词： Thermal conductivity of gases

Self-Supported Bifunctional P-Cose/Nf Electrodes for High Efficiency and Durability Hydrogen Production Coupled with Sulfion Valorization

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SSRN 2024年

作者： Qin, Shucan Peng, Qianqian Kong, Weizhen Xue, Rong Xu, Chongqing Shi, Jianming Liu, Yanrong Ma, Yunqian Jinan250353 China Longzihu New Energy Laboratory Zhengzhou Institute of Emerging Industrial Technology Henan University Zhengzhou450000 China Mingshuo Environment Group Weifang262605 China CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Mesoscience and Engineering Beijing Key Laboratory of Ionic Liquids Clean Process Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China

Integrating sulfide oxidation reaction (SOR) with hydrogen evolution reaction (HER) by electrochemical technology for sulfion valorization and hydrogen production is expected to maximize resources. Here, we report a phosphorus-doped transition metal selenide supported on nickel foam (P-CoSe/NF) to be efficiently and stably dual-used for SOR and HER, and this succulent-like catalyst with large surface area has an excellent activity up to 100 mA cm-2 at only 0.362 V. The H2 Faraday efficiency and rate of sulfur evolution reach 97.4% and 26.24 mg h-1, respectively. The Density Functional Theory calculations demonstrate that P-doping can offer an optimal electronic structure and local coordination environment by tuning d electron number. The potential rate-limiting step with a low energy barrier indicates the self-cleaning tendency. This work presents a promising approach for transition metal selenide catalysts in the electrochemistry field, representing a significant advancement in low-cost and high value-added utilization of waste resources. © 2024, The Authors. All rights reserved.

关键词： Hydrogen production

Metabolic Mechanism of P-Cresol Biodegradation by Bacillus Subtilis Zw: Coexistence of Diverse Metabolic Pathways

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SSRN 2024年

作者： Wang, Xueting Liu, Shihao Ding, Xiaoke Zhang, Lele Lv, Xueru Li, Jie Song, Caihong Zhang, Chen Wang, Shenghui College of Life Science Liaocheng University Liaocheng252059 China State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China

The aromatic compound p-cresol is a notorious industrial pollutant characterized by its high toxicity, persistence and bioaccumulation within higher organisms. A thorough understanding of the microbial metabolic pathways involved in p-cresol degradation is critical for the design and optimization of microbial wastewater treatment systems. Despite numerous studies on the degradation pathways of p-cresol by various microbial species, the metabolic diversity within a single strain remains largely unexplored. This study investigated the metabolic mechanism of p-cresol in Bacillus subtilis ZW, a bacterium capable of degrading p-cresol. Through LC-MS analysis, we identified twelve distinct metabolic intermediates in the culture of strain ZW, leading to the proposal of three plausible degradation pathways. These include methyl hydroxylation, direct aromatic ring hydroxylation, and phosphorylation of the hydroxyl group, and all of which may concurrently contribute to p-cresol biodegradation by strain ZW. Further study showed that the genome of strain ZW harbored 47 coding genes associated with the degradation of p-cresol and its structural analogs, underscoring the metabolic versatility of this strain and its potential for xenobiotic biodegradation. These findings contribute valuable insights into the biodegradation mechanisms of pollutants. Under optimal degradation conditions of 35 °C and pH 7.0, strain ZW demonstrated the capacity to metabolize 27.5% of p-cresol (10 mg/L) in minimal salt media within a week, and was capable of completely degrading 10 mg/L p-cresol in wastewater within five days. The potential utility of strain ZW in the bioremediation of p-cresol and other aromatic compounds is thus evident. © 2024, The Authors. All rights reserved.

关键词： Aromatization

Palladium-Catalyzed Dicarbonylation of 1,3-Butadiene and the Mechanisms of Catalyst Deactivation

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SSRN 2023年

作者： Zhang, Peng Zhang, Penghe Wang, Liwen Xin, Jiayu Han, Lijun Liu, Zhichang Hu, Yufeng Zhao, Hui Yan, Ruiyi Zhang, Shu College of Engineering and Environment China University of Petroleum Beijing102249 China CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex Systems Beijing Key Laboratory of Ionic Liquids Clean Process Innovation Academy for Green Manufacture CAS Beijing100190 China

The dicarbonylation of 1,3-butadiene (BD) offers a more environmentally friendly pathway for the industrial development of adipate diesters. However, the catalytic mechanism of this reaction and the stability of the catalytic system have not received much attention. Herein, the kinetics of dicarbonylation of BD in a homogeneous Pd(TFA)2/1,2-di-tert-butyl phosphoxane (dtbpx)/p-TsOH (PTSA) catalytic system was investigated. Based on the kinetic study, a possible reaction mechanism for the dicarbonylation of BD was proposed. 31P-NMR, ICP, ESI-MS, and IR were applied to gain insights into the complexity of the deactivation of the Pd(TFA)2/dtbpx/PTSA catalytic system. It is found that the Pd(TFA)2/dtbpx catalytic system is unstable in the presence of acid, and the dtbpx ligand is readily oxidized and protonated and thus loses its ability to coordinate with Pd(0), leading to Pd(0) inactivation by aggregation. In addition, the catalytic system deactivation pathway was postulated. Density-functional theory (DFT) calculations reveal that CO can coordinate with the complex [(dtbpx)Pd] to lower its coordination energy which leads to the decomposition of the complex [(dtbpx)Pd] and affects the stability of the catalytic system. Furthermore, the complex [(dtbpx)Pd] has a very low polymerization energy, which implies that [(dtbpx)Pd] has a strong tendency to self-polymerize. © 2023, The Authors. All rights reserved.

关键词： Density functional theory

Pickering interfacial biocatalysis with enhanced diffusion processes for CO_(2) mineralization

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Chinese Journal of Catalysis 2022年第4期43卷 1184-1191页

作者： Boyu Zhang Jiafu Shi Yang Zhao a Han Wang Ziyi Chu Yu Chen Zhenhua Wu Zhongyi Jiang School of Environmental Science&Engineering Tianjin UniversityTianjin 300072China Collaborative Innovation Center of Chemical Science and Engineering(Tianjin) Tianjin 300072China State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Utilization of carbon dioxide(CO_(2))has become a crucial and anticipated solution to address environmental and ecological *** such as carbonic anhydrase(CA)can efficiently convert CO_(2) into various platform chemicals under ambient conditions,which offers a promising way for CO_(2) ***,we constructed a Pickering interfacial biocatalytic system(PIBS)stabilized by CA‐embedded MOFs(ZIF‐8 and ZIF‐L)for CO_(2) *** structure engineering of MOFs and incorporation of Pickering emulsion,the internal and external diffusion processes of CO_(2) during the enzymatic mineralization were greatly *** CO_(2) was ventilated at a flow rate of 50 mL min^(–1) for 1 h,the pH value of PIBS dropped from~8.00 to~6.50,while the average pH value of free system only dropped to~7.15,indicating that the initial reaction rate of CO_(2) mineralization of PIBS is nearly twice that of the free *** the 8^(th) cycle reaction,PIBS can still produce more than 9.8 mg of CaCO_(3) in 5 min,realizing efficient and continuous mineralization of CO_(2).

关键词： Carbon dioxide conversion Carbonic anhydrase Pickering emulsion Metal‐organic frameworks Diffusion intensification

A facile ionic liquid approach to prepare cellulose fiber with good mechanical properties directly from corn stalks

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green Energy & Environment 2020年第2期5卷 223-231页

作者： Jiming Yang Xingmei Lu Yanqiang Zhang Junli Xu Yongqing Yang Qing Zhou Beijing Key Laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and EngineeringState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing100049China

It is very difficult to directly spin the lignocellulose without *** liquids(ILs)are promising solvent to dissolve lignocellulose to prepare cellulose ***,the degree of cellulose polymerization(DP)is reduced when lignocellulose is dissolved in ILs,and the lignin removal rate is *** elongation at break and tensile strength of the fibers obtained by spinning the lignocellulose dissolved in ILs are *** this paper,preparing cellulose fiber directly from lignocellulose based on dissolving corn stalk via[C4mim]Cl-L-arginine binary system is *** shows that the removal rate of lignin can reach 92.35%and the purity of cellulose can reach 85.32%after corn stalk was dissolved at 150℃C for 11.5 h when the mass fraction of arginine is 2.5%.The elongation at break of fiber reached 10.12%and the tensile strength reached 420 *** is mainly due to the fact that L-arginine not only inhibits the degradation of cellulose but also promotes the *** any pulping or pretreatment,preparing cellulose fibers via direct dissolution and extrusion may provide a simple and effective way to prepare many novel cellulose materials.

关键词： Cellulose fibers Ionic liquids Corn stalks Dissolving Directly spinning

Modification to solution-diffusion model for performance prediction of nanofiltration of long-alkyl-chain ionic liquids aqueous solutions based on ion cluster

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green Energy & Environment 2020年第1期5卷 105-113页

作者： Jianguo Qian Ruiyi Yan Xiaomin Liu Chunshan Li Xiangping Zhang Key Laboratory of Green Process and Engineering Beijing Key Laboratory of Ionic Liquids Clean ProcessState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China College of Chemistry and Chemical Engineering University of Chinese Academy of SciencesBeijing100049China

Mathematical modeling for nanofiltration of ionic liquids(ILs) solutions could assist to understand transfer mechanism and predict experimental values. In this work, modeling by solution-diffusion model for nanofiltration of long-alkyl-chain ILs aqueous solutions was proposed. Molecular simulations were performed to validate the existence of ion cluster in long-alkyl-chain ILs aqueous solution. Based on the results of simulations, parameters used in the solution-diffusion model were modified, such as concentration of ILs and diameter of ion *** modeling process was developed for three long-alkyl-chain ILs aqueous solutions with different concentrations(1-alkyl-3-methylimidazolium chloride: [C6 mim]Cl, [C8 mim]Cl, [C10 mim]Cl). The calculated values obtained from modified solution-diffusion model could well match the experimental values.

关键词： Solution-diffusion model Nanofiltration Long-alkyl-chain ionic liquid Molecular dynamic simulation Ion cluster

Heteronuclear Bicentric Ionic Liquids Tailored for Mild Catalytic Conversion of Co2 into Cyclic Carbonates

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SSRN 2024年

作者： Shabbir, Irfan Ndayambaje, Jean Damascene Dong, Li Su, Qian Cheng, Weiguo CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex Systems Beijing Key Laboratory of Ionic Liquids Clean Process Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China University of Chinese Academy of Sciences Beijing100049 China Zhengzhou Institute of Emerging Industrial Technology Henan Zhengzhou450000 China

The rapid increase of CO2 in the environment is creating severe climate catastrophes and rising ocean surfaces. Therefore, its reduction and green utilization into value-added materials is significant. Herein, heteronuclear bicentric pyridinium-based ionic liquids (BPyILs) tailored with different chain lengths and halogen anions have been synthesized and structurally characterized. The BPyILs were utilized as thermally stable, metal-free, and homogeneous catalysts to synthesize other cyclic organic carbonates (COCs) using various epoxides and sustainable, economical, and inert CO2, and their catalytic activity phenomenon has been discussed in detail. The results demonstrated that [TMGH+][ ̶O2MPy+][Br ̶] possesses Lewis acid-base bifunctional characteristics with strong nucleophilic active sites, which play an essential synergistic effect on the activation of CO2 and the ring-opening of epoxides. Various factors affecting the conversion and selectivity of catalysts, including reaction temperature, halide ion, catalyst amount, CO2 pressure, and reaction time, were further investigated. The results illustrated that under metal and solvent-free conditions, dual functionalized bicentric PyILs ([TMGH+][ ̶O2MPy+][Br ̶]) exhibited 99.7 % COC yield and 99.9 % selectivity at 90 oC temperature and 1 MPa CO2 pressure up to 4 h for the cycloaddition reaction between CO2 and propylene oxide (PO). At the same time, the turn-over frequency was as high as 10.1 h-1. Moreover, the versatility and recyclability of the catalyst were studied, and a plausible reaction mechanism was proposed. Compared to previously reported functionalized bicentric catalysts, [TMGH+][ ̶ O2MPy+][Br ̶ ] requires mild reaction conditions without using any metal, solvent, or co-catalyst, which demonstrates the bright prospect of synthesizing pyridinium-based bicentric (BPyILs) catalysts and its practical use in CO2 conversion, activation, and utilization. © 2024, The Authors. All rights reserved.

关键词： Ionic liquids

Intensifying Electron Utilization by Surface-Anchored Rh Complex for Enhanced Nicotinamide Cofactor Regeneration and Photoenzymatic CO_(2)Reduction

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Research 2021年第1期2021卷 507-517页

作者： Yuqing Cheng Jiafu Shi Yizhou Wu Xueying Wang Yiying Sun Ziyi Cai Yu Chen Zhongyi Jiang Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin University92 Weijin RoadNankai DistrictTianjin 300072China Collaborative Innovation Center of Chemical Science and Engineering(Tianjin) 92 Weijin RoadNankai DistrictTianjin 300072China School of Environmental Science&Engineering Tianjin University92 Weijin RoadNankai DistrictTianjin 300072China State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 10090China

Solar-driven photocatalytic regeneration of cofactors,including reduced nicotinamide adenine dinucleotide(NADH),reduced nicotinamide adenine dinucleotide phosphate(NADPH),and reduced flavin adenine dinucleotide(FADH_(2)),could ensure the sustainable energy supply of enzymatic reactions catalyzed by oxidoreductases for the efficient synthesis of ***,the elevation of cofactor regeneration efficiency is severely hindered by the inefficient utilization of electrons transferred on the surface of *** by the phenomenon of ferredoxin-NADP+reductase(FNR)anchoring on thylakoid membrane,herein,a homogeneous catalyst of rhodium(Rh)complex,[Cp_(∗)Rh(bpy)H_(2)O]^(2+),was anchored on polymeric carbon nitride(PCN)mediated by a tannic acid/polyethyleneimine(TA/PEI)adhesive layer,acquiring PCN@TA/PEI-Rh core@shell *** by visible light,electrons were excited from the PCN core,then transferred through the TA/PEI shell,and finally captured by the surface-anchored Rh for instant utilization during the regeneration of *** TA/PEI-Rh shell could facilitate the electron transfer from the PCN core and,more importantly,achieved~1.3-fold elevation of electron utilization efficiency compared with ***,the PCN@TA/PEI-Rh afforded the NADH regeneration efficiency of 37.8%after 20 min reaction under LED light(405 nm)illumination,over 1.5 times higher than PCN with free *** of the NADH regeneration system with formate dehydrogenase achieved continuous production of formate from carbon dioxide(CO_(2)).Our study may provide a generic and effective strategy to elevate the catalytic efficiency of a photocatalyst through intensifying the electron utilization.

关键词： enzymatic dinucleotide catalyst