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Efficient hydrogenation of ethylene carbonate derived from CO_(2) to synthesize methanol and ethylene glycol over core-shell Cu@GO catalyst

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Green Chemical Engineering 2022年第3期3卷 228-239页

作者： Chanjuan Zhang Liguo Wang Zhuo Han Peng He Yan Cao Jiachen Li Huiquan Li CAS Key Laboratory of Green Process and Engineering National Engineering Research Center of Green Recycling for Strategic Metal ResourcesInstitute of Process EngineeringChinese Academy of SciencesBeijing100190China Sino-Danish College University of Chinese Academy of SciencesBeijing100049China Sino-Danish Center for Education and Research University of Chinese Academy of SciencesBeijing100049China School of Chemical Engineering University of Chinese Academy of SciencesBeijing100049China Dalian National Laboratory for Clean Energy Dalian116023China

The synthesis of sustainable methanol and ethylene glycol(EG)via hydrogenation of ethylene carbonate(EC)has caught researchers’growing interests on account of the indirect chemical utilization of CO_(2).Core-shell Cu@GO catalysts with random nanoporous network of graphite oxide(GO)were synthesized via a simple method of ul-trasonic precipitation.Cu@GO catalysts were analyzed systematically by N_(2) physisorption,TGA measurement,XRD,FT-IR,Raman,TEM,SEM,and XPS(XAES).In particular,the mentioned method was confirmed to be effective to fabricate the high dispersity core-shell Cu@GO catalysts through promoting the specific surface area.The as-prepared Cu@GO catalyst was then successfully applied in the hydrogenation of CO_(2)-derived EC to pro-duce methanol and EG.A high TOF of 1526 mg EC g cat^(-1) h^(-1) could be attained in EC hydrogenation at the reaction temperature of 493K.Accordingly,the correlation of catalytic structure and performance disclosed that the synergistic effect between Cu^(+) and Cu^(0) was responsible for achieving high activity of the catalyst.In addition,the reusability of Cu@GO catalyst suggested that graphite oxide shell structure could decrease the aggregation of Cu particles,thus enhance the stability of Cu-based catalysts.DFT calculation results suggested that the involvement of carbon film on Cu was favorable for the stabilization of the active sites.This study is helpful for developing new and stable catalytic system for indirect chemical utilization of CO_(2) to synthesize commodity methanol and EG.

关键词： Ethylene carbonate Selective hydrogenation methanol Ethylene glycol Cu-based catalyst

methanol electro-oxidation to formate on iron-substituted lanthanum cobaltite perovskite oxides

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eScience 2022年第1期2卷 87-94页

作者： Fanxu Meng Chencheng Dai Zheng Liu Songzhu Luo Jingjie Ge Yan Duan Gao Chen Chao Wei Riccardo Ruixi Chen Jiarui Wang Daniel Mandler Zhichuan J.Xu School of Materials Science and Engineering Nanyang Technological University50 NanyangAvenueSingapore639798Singapore Energy Research Institute@NTU ERI@N Interdisciplinary Graduate SchoolTechnological UniversityNanyangSingapore639798Singapore Singapore-HUJ Alliance for Research and Enterprise NEW-CREATE Phase IICampus for Research Excellence and Technological Enterprise(CREATE)Singapore138602Singapore Institute of Chemistry The Hebrew University of JerusalemJerusalem9190401Israel

Electrochemically producing formate by oxidizing methanol is a promising way to add value to methanol.Noble metal-based electrocatalysts,which have been extensively studied for the methanol oxidation reaction,can catalyze the complete oxidation of methanol to carbon dioxide,but not the mild oxidation to formate.As a result,exploring efficient and earth-abundant electrocatalysts for formate production from methanol is of interest.Herein,we present the electro-oxidation of methanol to formate,catalyzed by iron-substituted lanthanum cobaltite(LaCo_(1-x)Fe_(x)O_(3)).The Fe/Co ratio in the oxides greatly influences the activity and selectivity.This effect is attributed to the higher affinity of Fe and Co to the two reactants:CH3OH and OH,respectively.Because a balance between these affinities is favored,LaCo_(0.5)Fe_(0.5)O_(3) shows the highest formate production rate,at 24.5 mmol h^(-1) g_(oxide)^(-1),and a relatively high Faradaic efficiency of 44.4%in a series of(LaCo_(1-x)Fe_(x)O_(3))samples(x=0.00,0.25,0.50,0.75,1.00)at 1.6 V versus a reversible hydrogen electrode.

关键词： methanol Electro-oxidation Formate Oxides Perovskite

CO_(2) hydrogenation to methanol over Rh/In_(2)O_(3)–ZrO_(2)catalyst with improved activity

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Green Chemical Engineering 2022年第2期3卷 165-170页

作者： Zhe Lu Jing Wang Kaihang Sun Shilong Xiong Zhitao Zhang Chang-jun Liu School of Chemical Engineering and Technology Tianjin UniversityTianjin300072China

The In_(2)O_(3)supported rhodium catalyst has been previously confirmed to be active for CO_(2)hydrogenation to methanol.In this work,the In_(2)O_(3)–ZrO_(2)solid solution was prepared and employed to support the rhodium catalyst.The deposition-precipitation method was applied to make the Rh catalyst highly dispersed.The catalyst characterization confirms that the use of ZrO_(2)optimizes and stabilizes the oxygen vacancies of In_(2)O_(3),which causes the enhanced adsorption and activation of CO_(2).The highly dispersed Rh catalyst remarkably improves the hydrogenation ability of the In_(2)O_(3)–ZrO_(2)support.Compared to Rh/In_(2)O_(3),the In_(2)O_(3)–ZrO_(2)supported Rh catalyst shows significantly higher activity with high methanol selectivity.For instance,at 300℃ and 5 MPa,the methanol selectivity over Rh/In_(2)O_(3)–ZrO_(2)reaches 66.5%with a space-time yield(STY)of methanol of 0.684 g MeOH h^(-1) g cat-1 and a CO_(2)conversion of 18.1%.The methanol selectivity and methanol STY at 300℃ is 19% and 26% higher than that of the Rh/In_(2)O_(3)catalyst.

关键词： Rh In_(2)O_(3) ZrO_(2) CO_(2) Hydrogenation methanol

Direct conversion of methane to methanol by electrochemical methods

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Green Energy & Environment 2022年第6期7卷 1132-1142页

作者： Haomin Jiang Luting Zhang Zhiwei Han Yang Tang Yanzhi Sun Pingyu Wan Yongmei Chen Morris D.Argyle Maohong Fan Institute of Applied Electrochemistry College of ChemistryBeijing University of Chemical TechnologyBeijing100029China Department of Chemical Engineering Brigham Young UniversityProvoUT84602USA College of Engineering and Applied Sciences School of Energy ResourcesUniversity of WyomingLaramieWY82071USA

A convenient method for methane(CH_(4))direct conversion to methanol(CH_(3)OH)is of great significance to use methane-rich resources,especially clathrates and stranded shale gas resources located in remote regions.Theoretically,the activation of CH_(4) and the selectivity to the CH_(3)OH product are challenging due to the extreme stability of CH_(4) and relatively high reactivity of CH_(3)OH.The state-of-the-art‘methane reforming-methanol synthesis’process adopts a two-step strategy to avoid the further reaction of CH_(3)OH under the harsh conditions required for CH_(4) activation.In the electrochemical field,researchers are trying to develop conversion pathways under mild conditions.They have found suitable catalysts to activate the C–H bonds in methane with the help of external charge and have designed the electrode reactions to continuously generate certain active oxygen species.These active oxygen species attack the activated methane and convert it to CH_(3)OH,with the benefit of avoiding over-oxidation of CH_(3)OH,and thus obtain a high conversion efficiency of CH_(4) to CH_(3)OH.This mini-review focuses on the advantages and challenges of electrochemical conversion of CH4 to CH_(3)OH,especially the strategies for supplying electro-generated active oxygen species in-situ to react with the activated methane.

关键词： Methane methanol Direct conversion Electrochemical methods Active oxygen species

Selective Oxidation of Methane into methanol Under Mild Conditions

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Chemical Research in Chinese Universities 2022年第3期38卷 671-676页

作者： LIU Yifeng WANG Liang XIAO Feng-Shou Key Lab of Applied Chemistry of Zhejiang Province Department of ChemistryZhejiang UniversityHangzhou310028P.R.China Key Lab of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou310027P.R.China Zhejiang Tianlan Environmental Protection Technology Limited Company Hangzhou310012P.R.China

Selective oxidation of methane to methanol under mild conditions has been considered as a dream reaction but suffers from poor efficiency due to the strong C-H bond of methane and easy overoxidation of the methanol product.For overcoming these problems,a series of strategies has been developed for improving methanol productivity with oxidants of hydrogen peroxide and even a mixture of oxygen and hydrogen at mild temperatures.Significant achievements in these strategies using effective catalysts,such as supported metal nanoparticles,colloidal metal nanoparticles,and metal@zeolites are briefly concluded.Moreover,the current challenges,future perspectives for preparing active,selective,and stable catalysts,have been discussed.The zeolite fixed metal nanoparticle structure has been found to boost the reaction by benefiting the formation and enrichment of peroxide intermediates,which might guide the development of more efficient catalysts.

关键词： Methane oxidation Metal@zeolite Hydrogen peroxide methanol

Analysis of routes for electrochemical conversion of CO_(2) to methanol

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Clean Energy 2022年第1期6卷 202-210页

作者： Pingping Li Siqi Gong Chufu Li and Zhien Liu National Institute of Clean and low carbon Energy Beijing102209P.R.China

In the context of peak carbon and carbon neutrality,the utilization of CO_(2)has attracted attention with the aim of reducing carbon emissions by converting CO_(2)into high-value chemicals or energy.methanol(MeOH),which is both a hydrogen and a carbon carrier,is considered the most promising among the CO_(2)-conversion products.This paper focus on routes for electrochemical conversion of CO_(2)to MeOH using green power and green hydrogen to achieve negative CO_(2)emissions.Three feasible technical routes for electrochemical conversion of CO_(2)to MeOH are proposed in this paper:Route 1,electrolysis of water to H_(2)and hydrogenation of CO_(2)to MeOH;Route 2,electrochemical reduction of CO_(2)to MeOH;and Route 3,co-electrolysis of CO_(2)-H_(2)O to syngas and synthesis of MeOH from syngas.Techno-economic assessments of the three routes are conducted using technical maturity surveys,system simulations and cost analyses to provide reference data for route selection for CO_(2)conversion to MeOH in China.Compared with the other routes,Route 1 is advantageous in terms of technical maturity and commercial application prospects.Although Route 1 is presently economically unviable,it is expected to achieve profitability and commercial application in the future with decreases in the cost of renewable power and continuous development of water-electrolysis technology.

关键词： CO_(2) electrolysis hydrogenation carbon capture and utilization methanol electrochemical conversion carbon neutrality

Outbreak of methanol-induced optic neuropathy in early COVID-19 era;effectiveness of erythropoietin and methylprednisolone therapy

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World Journal of Clinical Cases 2023年第15期11卷 3502-3510页

作者： Seyed Ali Tabatabaei Mohammad Amini Ali A Haydar Mohammad Soleimani Kasra Cheraqpour Mansoor Shahriari Hossein Hassanian-Moghaddam Nasim Zamani Mohammad Reza AkbariDepartment of Ophthalmology Eye Research Center Farabi Eye Hospital Tehran University of Medical SciencesTehran ***Iran Department of Ophthalmology Imam Hossein Medical CenterShahid Beheshti University of Medical SciencesTehran ***Iran Department of Clinical Toxicology Shohada-e-Tajrish HospitalShahid Beheshti University of Medical SciencesTehran ***Iran Department of Internal Medicine StreetAgnes Medical CenterFresnoCA 93720United States

BACKGROUND methanol is a highly toxic,non-potable alcohol.Outbreaks of methanol toxicity occur due to its fraudulent addition to alcoholic beverages as a cheaper substitute for ethanol.Recently,alongside the coronavirus disease 2019(COVID-19)pandemic,rumors circulated on social media that consuming alcohol can prevent or cure the virus,leading to a COVID-19 and methanol-induced optic neuropathy(MON)syndemic.AIM To investigate the impact of erythropoietin(EPO)on the outcomes of patients diagnosed with MON.METHODS In this prospective study,105 patients presenting with acute bilateral visual loss secondary to methanol intoxication were enrolled from March to May 2020 at Farabi Eye Hospital.A comprehensive ocular examination was conducted for all participants.Recombinant human EPO and methylprednisolone were administered intravenously to all patients for three consecutive days.RESULTS The mean age of the participants was 39.9 years(±12.6).Ninety-four patients were male and eleven were female.The mean pre-treatment best corrected visual acuity(BCVA)improved from 2.0±0.86 to 1.39±0.69 logarithm of the minimum angle of resolution post-treatment(Pmethanol toxicity in the current COVID-19 era.

关键词： Alcohol Ethanol methanol Optic neuropathy Erythropoietin COVID-19

Controlled location of S vacancies in MoS_(2) nanosheets for high-performance hydrogenation of CO_(2) to methanol

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Journal of Energy Chemistry 2022年第1期31卷 113-115,I0004页

作者： Gabriele Centi Dept.ChiBioFarAm University of MessinaItaly and ERIC Aisbl.BrusselsBelgium

Introduction In a joint contribution among many Chinese research Institutes,a recent paper published on Nature Catalysis reported the use of sulfur vacancy-rich MoS_(2)as a novel catalyst for the hydrogenation of CO_(2)to methanol[1].A commentary on this paper was also published on the same journal[2]reporting as a summary:"Highly active,selective and stable catalysts for the hydrogenation ofC0_(2)to methanol are immensely sought after.Now,using a broad range of spectroscopic methods,in-plane double sulfur vacancies of MoS_(2)sheets have been suggested to catalyse this reaction using an unusual mechanism".

关键词： CO_(2) methanol MOS_(2)nanosheet In-plane S vacancies

Seminal HPV detection:a pilot study comparing the preservation effectiveness and cost between a methanol-based solution and cryopreservation with liquid nitrogen

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Asian Journal of Andrology 2022年第5期24卷 560-561页

作者： Jynfiaf Francis Cecilia Kärrberg Jonas Hermansson Magnus Lindh Sofia Ganidou Ann Thurin-Kjellberg Kersti Lundin Randa Akouri Panagiotis Tsiartas Department of Reproductive Medicine Sahlgrenska University HospitalGothenburg 41345Sweden Department of Obstetrics and Gynecology Institute of Clinical SciencesSahlgrenska AcademyGothenburg UniversityGothenburg 40530Sweden Department of Research and Development Angered HospitalAngered 42465Sweden Department of Clinical Microbiology Sahlgrenska University HospitalGothenburg 41346Sweden Department of OncologyPathology Karolinska InstituteStockholm 17177Sweden

Dear Editor,Human papillomavirus(HPV)is the most common sexually transmitted virus worldwide,and high-risk HPV infection is the most important risk factor for cervical cancer.1 However,few conclusive data are available on the prevalence of the male HPV infection and its health consequences.It has been found that the prevalence of seminal HPV infection is higher in men with unexplained infertility,ranging between 10%and 35%compared with the general population(range:2%to 11%).2–4 In three recent systematic reviews,it was seen that HPV sperm infection may be associated with impaired sperm function that could lead to male infertility.2,4,5 HPV sperm infection with high-risk HPV among infertile men was shown to be associated with lower progressive sperm motility and higher DNA fragmentation index.6 Moreover,a high rate of pregnancy loss has been found among couples with HPV sperm infection after in vitro fertilization(IVF).7 In the majority of the studies performed to assess seminal HPV infection.

关键词： impaired methanol HPV