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Chemico-biological conversion of carbon dioxide

Journal of Energy Chemistry 2024年第2期89卷 371-387,I0009页

作者： Liangwei Hu Junzhu Yang Qi Xia Jin Zhang Hongxin Zhao Yuan Lu Zhejiang Province Key Laboratory of Plant Secondary Metabolism and Regulation College of Life Sciences and MedicineZhejiang Sci-Tech UniversityHangzhou 310018ZhejiangChina Key Laboratory of Industrial Biocatalysis Ministry of EducationTsinghua UniversityBeijing 100084China Department of Chemical Engineering Tsinghua UniversityBeijing 100084China College of Biological and Chemical Engineering Jiaxing UniversityJiaxing 314000ZhejiangChina

The unabated carbon dioxide(CO_(2))emission into the atmosphere has exacerbated global climate change,resulting in extreme weather events,biodiversity loss,and an intensified greenhouse effect.To address these challenges and work toward carbon(C)neutrality and reduced CO_(2)emissions,the capture and utilization of CO_(2)have become imperative in both scientific research and industry.One cutting-edge approach to achieving efficient catalytic performance involves integrating green bioconversion and chemical conversion.This innovative strategy offers several advantages,including environmental friendliness,high efficiency,and multi-selectivity.This study provides a comprehensive review of existing technical routes for carbon sequestration(CS)and introduces two novel CS pathways:the electrochemicalbiological hybrid and artificial photosynthesis systems.It also thoroughly examines the synthesis of valuable Cnproducts from the two CS systems employing different catalysts and biocatalysts.As both systems heavily rely on electron transfer,direct and mediated electron transfer has been discussed and summarized in detail.Additionally,this study explores the conditions suitable for different catalysts and assesses the strengths and weaknesses of biocatalysts.We also explored the biocompatibility of the electrode materials and developed novel materials.These materials were specifically engineered to combine with enzymes or microbial cells to solve the biocompatibility problem,while improving the electron transfer efficiency of both.Furthermore,this review summarizes the relevant systems developed in recent years for manufacturing different products,along with their respective production efficiencies,providing a solid database for development in this direction.The novel chemical-biological combination proposed herein holds great promise for the future conversion of CO_(2)into advanced organic compounds.Additionally,it offers exciting prospects for utilizing CO_(2)in synthesizing a wide range of industrial products.Ultimately,t

关键词： carbon dioxide Bioelectric synthesis Artificial photosynthesis Synthetic product

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Bimolecular reduction of carbon dioxide: double synthons for alkynes trifunctionalization

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Science China Chemistry 2024年第3期67卷 841-847页

作者： Wenfang Xiong Xiaobin Tan Hongjian Liu Baiyao Zhu Jinwu Zhao Jianxiao Li Chaorong Qi Huanfeng Jiang School of Pharmacy Guangdong Medical UniversityDongguan 523808China Key Lab of Functional Molecular Engineering of Guangdong Province School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China

carbon dioxide reduction, as a sustainable and versatile strategy for the access of chemical fuels, has attracted increasing attention and enormous efforts have been devoted to it in recent years. However, employing carbon dioxide as double synthons via bimolecular reduction remains challenging. Here, by leveraging the bimolecular reduction of carbon dioxide to carbonyl and methyl respectively, we describe a Pd-catalyzed trifunctionalization of alkynes with aryl iodide for the first time and showcase its advantages on the formation of various β-diketones and their application in the constructing of heterocyclic compounds with important biological activity, including pyrimidine, oxazole, pyrazole.

关键词： carbon dioxide bimolecular reduction trifunctionalization double synthons

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Finned Zn-MFI zeolite encapsulated noble metal nanoparticle catalysts for the oxidative dehydrogenation of propane with carbon dioxide

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Journal of Energy Chemistry 2023年第5期80卷 479-491,I0011页

作者： En-Hui Yuan Yiming Niu Xing Huang Meng Li Jun Bao Yong-Hong Song Bingsen Zhang Zhao-Tie Liu Marc-Georg Willinger Zhong-Wen Liu Key Laboratory of Syngas Conversion of Shaanxi Province School of Chemistry&Chemical EngineeringShaanxi Normal UniversityXi'an 7119ShaanxiChina Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016LiaoningChina College of Chemistry Fuzhou UniversityFuzhou 36108FujianChina National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230026AnhuiChina School of Natural Science(NAT) Department of ChemistryTechnical University of MunichLichtenbergstraje 485747 GarchingGermany

Oxidative dehydrogenation of propane with carbon dioxide(CO_(2)-ODP)characterizes the tandem dehydrogenation of propane to propylene with the reduction of the greenhouse gas of CO_(2)to valuable CO.However,the existing catalyst is limited due to the poor activity and stability,which hinders its industrialization.Herein,we design the finned Zn-MFI zeolite encapsulated noble metal nanoparticles(NPs)as bifunctional catalysts(NPs@Zn-MFI)for CO_(2)-ODP.Characterization results reveal that the Zn2+species are coordinated with the MFI zeolite matrix as isolated cations and the NPs of Pt,Rh,or Rh Pt are highly dispersed in the zeolite crystals.The isolated Zn2+cations are very effective for activating the propane and the small NPs are favorable for activating the CO_(2),which synergistically promote the selective transformation of propane and CO_(2)to propylene and CO.As a result,the optimal 0.25%Rh0.50%Pt@Zn-MFI catalyst shows the best propylene yield,satisfactory CO_(2)conversion,and long-term stability.Moreover,considering the tunable synergetic effects between the isolated cations and NPs,the developed approach offers a general guideline to design more efficient CO_(2)-ODP catalysts,which is validated by the improved performance of the bifunctional catalysts via simply substituting Sn4+cations for Zn2+cations in the MFI zeolite matrix.

关键词： Oxidative dehydrogenation Propane carbon dioxide Finned Zn-MFI zeolite Encapsulated noble metal nanoparticles

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Effects of zinc on χ-Fe_(5)C_(2) for carbon dioxide hydrogenation to olefins:Insights from experimental and density function theory calculations

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Chinese Journal of Chemical Engineering 2023年第2期54卷 206-214页

作者： Xianglin Liu Minjie Xu Chenxi Cao Zixu Yang Jing Xu State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China Maoming Branch R&D Institute SINOPECMaoming 525000China Key Laboratory of Smart Manufacturing in Energy Chemical Process Ministry of EducationEast China University of Science and TechnologyShanghai 200237China

Production of light olefins from CO_(2), the primary greenhouse gases, is of great importance to mitigate the adverse effects of CO_(2) emission on environment and to supply the value-added products from nonpetroleum resource. However, development of robust catalyst with controllable selectivity and stability remains a challenge. Herein, we report that Zn-promoted Fe catalyst can boost the stable and selective production of light olefins from CO_(2). Specifically, the Zn-promoted Fe exhibits a highly stable activity and olefin selectivity over 200 h time-on-stream compared to the unpromoted Fe catalyst, primarily owing to the preservation of active χ-Fe_(5)C_(2) phase. Structural characterizations of the spent catalysts suggest that Zn substantially regulates the content of iron carbide on the surface and suppresses the reoxidation of bulk iron carbide during the reaction. DFT calculations confirm that adsorption of surface carbon atoms and graphene-like carbonaceous species are not thermochemically favored on Zn-promoted Fe catalyst. carbon deposition by CAC coupling reactions of two surface carbon atoms and dehydrogenation of CH intermediate are also inhibited. Furthermore, the effects of Zn on antioxidation of iron carbide were also investigated. Zn favored the hydrogenation of surface adsorbed oxygen atoms to H_(2)O and the desorption of H_(2)O, which reduces the possibility of surface carbide being oxidized by the chemisorbed oxygen.

关键词： Reaction engineering χ-Fe_(5)C_(2) Zn promoter carbon dioxide Hydrogenation Density function theory

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Micro-interface enhanced mass transfer sodium carbonate absorption carbon dioxide reaction

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Chinese Journal of Chemical Engineering 2023年第12期64卷 208-223页

作者： Hu Shen Yingyu Xu Jigang An Bowen Jiang Jinnan Sun Guoqiang Yang Zhibing Zhang Key Laboratory of Mesoscopic Chemistry of Ministry of Education(MOE) School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Micro-interface intensified reactor(MIR)can be applied in series/parallel in the absorption of CO_(2)in industrial gases by Na_(2)CO_(3)due to the ability to produce large numbers of stable microbubbles.This work focuses on the variation pattern of mass transfer characteristics parameters of the reaction gas in Na_(2)CO_(3) solution under the influence of different solution properties and operating parameters in the reaction of CO_(2)absorption by Na2CO3.The mass transfer characteristics parameters include bubble Sauter mean diameter,gas holdup,interfacial area,liquid side mass transfer coefficient,and liquid side volume mass transfer coefficient kLa.The solution properties and operating parameters include Na2CO3 concentration(0.05–2.0 mol·L^(-1)),superficial gas velocity(0.00221–0.01989 m·s^(-1)),superficial liquid velocity(0.00332–0.02984 m·s^(-1)),and ionic strength(1.42456–1.59588 mol·kg^(-1)).And volumetric mass transfer coeffi-cients kLa and superficial reaction rates r of the MIR and the bubble column reactor are compared in the reaction of sodium carbonate absorption of carbon dioxide,and the former shows a greater improvement under different solution properties and operating parameters.The enhanced role of MIR in mass transfer in non-homogeneous reactions is verified and the feasibility of industrial practical applications of MIR is demonstrated.

关键词： carbon dioxide Absorption Microbubble Bubble Sauter mean diameter Interfacial area Mass transfer

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Reactive ball-milling synthesis of Co-Fe bimetallic catalyst for efficient hydrogenation of carbon dioxide to value-added hydrocarbons

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Journal of Energy Chemistry 2023年第9期84卷 210-218页

作者： Haipeng Chen Chenwei Wang Mengyang Zheng Chenlei Liu Wenqiang Li Qingfeng Yang Shixue Zhou Xun Feng College of Chemistry and Chemical Engineering Henan Key Laboratory of Function-Oriented Porous MaterialsLuoyang Normal UniversityLuoyang 471934HenanChina State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering Ningxia UniversityYinchuan 750021NingxiaChina College of Chemical and Biological Engineering Shandong University of Science and TechnologyQingdao 266590ShandongChina

Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-milling method for highly active and selective hydrogenation of CO_(2) to value-added hydrocarbons.When reacted at 320℃,1.0 MPa and 9600 mL h^(-1) g_(cat)^(-1),the selectivity to light olefin(C_(2)^(=)-C_(4)^(=)) and C_(5)+ species achieves 57.3% and 22.3%,respectively,at a CO_(2) co nversion of 31.4%,which is superior to previous Fe-based catalysts.The CO_(2) activation can be promoted by the CoFe phase formed by reactive ball milling of the Fe-Co_(3)O_(4) mixture,and the in-situ Co_(2)C and Fe_(5)C_(2) formed during hydrogenation are beneficial for the C-C coupling reaction.The initial C-C coupling is related to the combination of CO species with the surface carbon of Fe/Co carbides,and the sustained C-C coupling is maintained by self-recovery of defective carbides.This new strategy contributes to the development of efficient catalysts for the hydrogenation of CO_(2) to value-added hydrocarbons.

关键词： Reactive ball milling Co-Fe bimetallic catalyst carbon dioxide Value-added hydrocarbon C–C coupling reaction

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Paradoxical carbon dioxide embolism during laparoscopic hepatectomy without intracardiac shunt:A case report

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World Journal of Clinical Cases 2022年第9期10卷 2908-2915页

作者： Soeun Jeon Jeong-Min Hong Hyeon Jeong Lee Yesul Kim Hyunjong Kang Boo-young Hwang Dowon Lee Young-hoon Jung Department of Anesthesia and Pain Medicine Pusan National UniversitySchool of MedicineBusan 49241South Korea Biomedical Research Institute Pusan National University HospitalBusan 49241South Korea

BACKGROUND Laparoscopic hepatectomy has recently become popular because it results in less bleeding than open hepatectomy.However,CO_(2)embolism occurs more frequently.Most CO_(2)embolisms during laparoscopic surgery are self-resolving and non-symptomatic;however,severe CO_(2)embolism may cause hypotension,cyanosis,arrhythmia,and cardiovascular collapse.In particular,paradoxical CO_(2)embolisms are highly likely to cause neurological deficits.We report a case of paradoxical CO_(2)embolism found on transesophageal echocardiography(TEE)during laparoscopic hepatectomy,although the patient had no intracardiac shunt.CASE SUMMARY A 71-year-old man was admitted for laparoscopic left hemihepatectomy.During left hepatic vein ligation,the inferior vena cava was accidentally torn.We observed a sudden drop in oxygen saturation to 85%,decrease in systolic blood pressure(SBP)below 90 mm Hg,and reduction in end-tidal CO_(2)to 24 mm Hg.A“mill-wheel”murmur was auscultated over the precordium.The fraction of inspired oxygen was increased to 100%with 5 cm H2O of positive end-expiratory pressure(PEEP)and hyperventilation was maintained.Norepinephrine infusion was increased to maintain SBP above 90 mm Hg.A TEE probe was inserted,revealing gas bubbles in the right side of the heart,left atrium,left ventricle,and ascending aorta.The surgeon reduced the pneumoperitoneum pressure from 17 to 14 mm Hg and repaired the damaged vessel laparoscopically.Thereafter,the patient’s hemodynamic status stabilized.The patient was transferred to the intensive care unit,recovering well without complications.CONCLUSION TEE monitoring is important to quickly determine the presence and extent of embolism in patients undergoing laparoscopic hepatectomy.

关键词： carbon dioxide Embolism Laparoscopy Pneumoperitoneum Transesophageal echocardiography Case report

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Promotional nature of Sn on Pt/CeO_(2)for the oxidative dehydrogenation of propane with carbon dioxide

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Nano Research 2023年第5期16卷 6237-6250页

作者： Guo-Qing Yang Xing Ren Vita A.Kondratenko Heng-Bo Zhang Evgenii V.Kondratenko Zhong-Wen Liu Key Laboratory of Syngas Conversion of Shaanxi Province School of Chemistry&Chemical EngineeringShaanxi Normal UniversityXi’an 710119China Leibniz-Institut für Katalyse e.V Albert-Einstein-Strasse 29 aRostock 18059Germany

The oxidative dehydrogenation of propane with CO_(2)(CO_(2)-ODP)is a promising technology for the efficient production of propene in tandem with CO_(2)reduction to CO.However,the rational design of high-performance catalysts for this green process is still challenged by limited understanding of the nature of active sites and the reaction mechanism.In this work,the effects of SnO_(2) promoter on Pt/CeO_(2)activity and propene selectivity in CO_(2)-ODP are elucidated through varying the Sn/Pt molar ratio.When the ratio increases,propane conversion gradually decreases,while the propene selectivity increases.These dependences are explained by increasing the electron density of Pt through the promoter.The strength of this effect is determined by the Sn/Pt ratio.Owing to the electronic changes of Pt,CO_(2)-ODP becomes more favorable than the undesired CO_(2)reforming of propane.Sn-modified Pt–O–Ce bonds are reasonably revealed as the active sites for CO_(2)-ODP occurring through a redox mechanism involving the activation of CO_(2)over oxygen vacancies at Sn-modified Pt and CeO_(2)boundaries.These atomic-scale understandings are important guidelines for purposeful development of high-performance Pt-based catalysts for CO_(2)-ODP.

关键词： oxidative dehydrogenation carbon dioxide supported PtSn ceria

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Numerical Investigation of Jet Impingement Cooling with Supercritical Pressure carbon dioxide in a Multi-Layer Cold Plate during High Heat Flux

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Journal of Thermal Science 2023年第1期32卷 237-253页

作者： WEN Yaming LI Yulong LI Jingqi YU Xin-Gang National Key Laboratory of Science and Technology on Aero Engines Aero-Thermodynamics&Collaborative Innovation Center for Advanced Aero-Engine School of Energy and Power EngineeringBeihang UniversityBeijing 100191China Beijing Institute of Spacecraft System Engineering Beijing 100094China

Jet impingement cooling with supercritical pressure carbon dioxide in a multi-layer cold plate during the heat flux of 400 W/cm_(2) is investigated numerically.The generation and distribution of pseudocritical fluid with the high specific heat of supercritical pressure carbon dioxide and the mechanism of the heat transfer enhancement led by the high specific heat are analyzed.For a given nozzle diameter,the effects of the geometric parameters of a multi-layer cold plate such as the relative nozzle-to-plate distance,relative plate thickness,and relative upper fluid thickness on the average heat transfer coefficient are studied.The results show that the target surface is cooled effectively with supercritical pressure carbon dioxide jet impingement cooling.When the radial distance is less than 6 mm,the maximum wall temperature is 368 K,which is 30 K lower than the maximum junction temperature for a silicon-based insulated gate bipolar transistor,a typical electronic power device.There is a pseudocritical fluid layer near the target surface,where specific heat reaches above 34 kJ/(kg·K)locally.The drastic rise of the specific heat leads to obvious heat transfer enhancement.Within a certain range,the local heat transfer coefficient and the specific heat are linearly correlated and Stanton number remains constant over this range.The heat transfer coefficient is at a maximum when the relative nozzle-to-plate distance is 1.As the relative plate thickness increases from 0.5 to 3.5 or the relative upper fluid thickness increases from 0.5 to 2.5,the average heat transfer coefficient decreases monotonically.

关键词： high heat flux jet impingement cooling supercritical pressure carbon dioxide heat transfer enhancement

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Zn_(x)Zr/HZSM-5 as efficient catalysts for alkylation of benzene with carbon dioxide

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Frontiers of Chemical Science and Engineering 2023年第4期17卷 404-414页

作者： Junjun Cheng Yitao Zhao Guohao Xu Peng Zhang Xuedong Zhu Fan Yang Engineering Research Center of Large-Scale Reactor Engineering and Technology Ministry of EducationEast China University of Science&TechnologyShanghai 200237China

Alkylation of benzene with carbon dioxide and hydrogen to produce toluene and xylene could increase the added-value of surplus benzene as well as relieve environmental problems like green-house effect.In this work,the alkylation benzene with carbon dioxide and hydrogen reaction was proceeded by using the mixture of zinc-zirconium oxide and HZSM-5 as bifunctional catalyst.The equivalent of Zn/Zr=1 displays the best catalytic performance at 425℃ and 3.0 MPa,and benzene conversion reaches 42.9%with a selectivity of 90%towards toluene and xylene.Moreover,the carbon dioxide conversion achieves 23.3%and the carbon monoxide selectivity is lower than 35%,indicating that more than 50%carbon dioxide has been effectively incorporated into the target product,which is the best result as far as we know.Combined with characterizations,it indicated that the Zn and Zr formed a solid solution under specific conditions(Zn/Zr=1).The as-formed solid solution not only possesses a high surface area but also provides a large amount of oxygen vacancies.Additionally,the bifunctional catalyst has excellent stabilities that could keep operating without deactivation for at least 80 h.This work provides promising industrial applications for the upgrading of aromatics.

关键词： carbon dioxide alkylation of benzene solid solution catalyst bifunctional catalyst

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