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Electrochemical conversion of methane to bridge the gap in the artificial carbon cycle

Journal of energy Chemistry 2025年第1期100卷 286-308页

作者： Yuhao Peng Yuefeng Song Ihar Razanau Juanxiu Xiao Wei Xiao Di Hu Guoxiong Wang College of Chemistry and Molecular Sciences Hubei Key Laboratory of Electrochemical Power Sources Wuhan University State key laboratory of Catalysis Dalian National Laboratory for Clean Energy iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Dalian Institute of Chemical Physics Chinese Academy of Sciences laboratory of Physical-Chemical Technologies SSPA Scientific and Practical Materials Research Centre of NAS of Belarus State key laboratory of Marine Resources utilization in South China Sea Collaborative Innovation Center of Marine Science and Technology School of Marine Science and Engineering Hainan University Department of Chemical and Environmental Engineering University of Nottingham Ningbo China

Methane, an abundant one-carbon（C1） resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO2emissions and coke deposition. Electrochemical conversion of methane（ECM） using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO2emission.

关键词： Methane Electrochemical conversion Reaction mechanism Catalyst design Electrode Electrocatalysis

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Gas-Solid Flow,Combustion Characteristics,and Gas Emissions in a 75 t/h CFB Boiler Based on the CPFD Method

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Journal of Thermal Science 2025年第1期 323-336页

作者： HUANG Xiankun BAI Zhang ZHU Xiaoli WANG Shuoshuo MU Lin GONG Liang College of New energy China University of Petroleum (East China) key laboratory of ocean energy utilization and energy Conservation of Ministry of Education School of Energy and Power EngineeringDalian University of Technology

A 3D simulation using Computational Particle Fluid Dynamics（CPFD） methods was used to calculate coal combustion in a 75 t/h industrial-scale circulating fluidized bed（CFB） *** characteristics,gas-solid flow characteristics,and gaseous pollutant emissions of CFB boilers from combustion ignition to stable operation were systematically evaluated in this *** show that the temperature distribution is relatively uniform throughout the *** the combustion process unfolds within the boiler,the gas composition curve strikingly portrays the inverse correlation between CO2and *** the combustion reaction progresses,it becomes evident that the concentration of CO2progressively increases,while the concentration of O2concurrently *** inverse relationship underscores the fundamental combustion reaction,where carbon-based fuels react with oxygen to produce carbon dioxide and release ***,a comprehensive analysis has revealed that,from ignition to stable combustion,both nitric oxide（NO） and sulfur dioxide（SO2） emissions exhibit a declining *** reduction in pollutant generation is attributed to the improvement in combustion *** complete combustion leads to lower levels of unburned hydrocarbons,which are prone to NO ***,the sulfur content in the fuel is more efficiently oxidized to sulfur trioxide（SO3） or bound in sulfates,reducing *** steady state in the simulation,the SO2mass flow rate varies significantly with the furnace height,gradually increasing from 0.07 kg·s-1at 4 m at the bottom of the furnace to a peak of 0.078 kg·s-1at 8 m in the center,and then decreasing to 0.06 kg·s-1at 20m at the top of the furnace.

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Identifying the dynamic behaviors in complete reconstruction of Co-based complex precatalysts during electrocatalytic oxygen evolution

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Journal of energy Chemistry 2025年第1期100卷 226-233页

作者： Jingfang Zhang Danyang Wu Linke Cai Youluan Lu Fanpeng Cheng Lijuan Shi Qun Yi Yao Liu Yi Huang key laboratory of Green Chemical Engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education Hubei Key Laboratory of Novel Reactor and Green Chemical Technology School of Chemical Engineering & Pharmacy Wuhan Institute of Technology key laboratory of Pesticide & Chemical Biology of Ministry of Education Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of Education College of Chemistry Central China Normal University College of Materials Science and Engineering Fuzhou University

Transition metal-based nanomaterials have emerged as promising electrocatalysts for oxygen evolution reaction（OER）. Considerable research efforts have shown that self-reconstruction occurs on these nanomaterials under operating conditions of OER process. However, most of them undergo incomplete reconstruction with limited thickness of reconstruction layer, leading to low component utilization and arduous exploration of real catalytic mechanism. Herein, we identify the dynamic behaviors in complete reconstruction of Co-based complexes during OER. The hollow phytic acid（PA） cross-linked CoFe-based complex nanoboxes with porous nanowalls are designed because of their good electrolyte penetration and mass transport ability, in favor of the fast and complete reconstruction. A series of experiment characterizations demonstrate that the reconstruction process includes the fast substitution of PA by OH-to form Co（Fe）(OH)xand subsequent potential-driven oxidation to Co（Fe）OOH. The obtained CoFeOOH delivers a low overpotential of 290 mV at a current density of 10 mA cm-2and a long-term *** experiment results together with theory calculations reveal that the Fe incorporation can result in the electron rearrangement of reconstructed CoFeOOH and optimization of their electronic structure,accounting for the enhanced OER activity. The work provides new insights into complete reconstruction of metal-based complexes during OER and offers guidelines for rational design of high-performance electrocatalysts.

关键词： Complete reconstruction Co-based complex Precatalysts Oxygen evolution reaction

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Interfacial Zn2+-solvation regulator towards reversible and stable Zn anode

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Journal of energy Chemistry 2025年第1期100卷 684-692页

作者： Miao Zhou Xiongbin Luo Hang Li Shan Guo Zhuang Tong Xiaotao Zhou Xu Li Zhaohui Hou Shuquan Liang Guozhao Fang College of Mechanical Engineering Key Laboratory of Hunan Province for Advanced Carbon-based Functional Materials Hunan Institute of Science and Technology School of Materials Science and Engineering Key Laboratory of Electronic Packaging and Advanced Functional Materials of Hunan Province Central South University College of Materials and Metallurgy Guizhou University National energy Metal Resources and New Materials key laboratory Central South University

Aqueous zinc-ion batteries （AZIBs） are fundamentally challenged by the instability of the electrode/electrolyte interface,predominantly due to irreversible zinc （Zn） deposition and hydrogen ***,the intricate mechanisms behind the electrochemical discrepancies induced by interfacial Zn2+-solvation and deposition behavior demand comprehensive *** molecules endowed with special functional groups （such as hydroxyl,carboxyl,etc.） have the potential to significantly optimize the solvation structure of Zn2+and regulate the interfacial electric double layer （EDL）.By increasing nucleation overpotential and decreasing interfacial free energy,these functional groups facilitate a lower critical nucleation radius,thereby forming an asymptotic nucleation model to promote uniform Zn ***,this study presents a pioneering approach by introducing trace amounts of n-butanol as solvation regulators to engineer the homogenized Zn （H-Zn） anode with a uniform and dense *** interfacial reaction and structure evolution are explored by in/ex-situ experimental techniques,indicating that the H-Zn anode exhibits dendrite-free growth,no by-products,and weak hydrogen evolution,in sharp contrast to the bare ***,the H-Zn anode achieves a remarkable Zn utilization rate of approximately 20% and simultaneously sustains a prolonged cycle life exceeding 500 ***,the H-Zn//NH4V4O10（NVO） full battery showcases exceptional cycle stability,retaining 95.04%capacity retention after 400 cycles at a large current density of 5 A *** study enlightens solvation-regulated additives to develop Zn anode with superior utilization efficiency and extended operational lifespan.

关键词： Aqueous zinc-ion batteries Interfacial reaction Asymptotic nucleation model Reversible and stable Zn anode

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Synergistic promotion strategy of “dual-site” and “dual-path” to enhance the C–C coupling between CO2 and HCHO driven by photoelectrocatalysis

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Journal of energy Chemistry 2025年第1期100卷 39-49页

作者： Hongqiang Yang Jianfeng Zheng Guoyu Wang Yifei Gao Yatao Yang Jia Li Xiaojin Han Yan Cui Zhanggen Huang National key laboratory of High Efficiency and Low Carbon utilization of Coal Institute of Coal Chemistry Chinese Academy of Science University of Chinese Academy of Science Shenyang University of Chemical Technology

Photoelectrocatalytic coupling CO2and volatile organic compounds （VOCs） is a promising green strategy for the synergistic conversion of the two carbon-containing resources to *** catalytic efficiency is always at the mercy of chemical inertness of CO2and the competitive hydrogen evolution of ***,a modified g-C3N4/ZnAl-LDH Z-scheme heterojunction catalyst with dual reaction site was rationally designed and precisely *** Faraday efficiency of ethanol reached 68.67%with a corresponding formation rate of 227.3μmol *** revealed by in-situ characterizations and density functional theory calculations,CO2and HCHO were absorbed at Zn site and N site,***,*CO generated from CO2and HCHO was converted to*CH3O and*CHO on the dual-active-site *** detailed reaction mechanism experiments indicated that C–C coupling only occurred between*CO and*CH3O in electrocatalysis *** from the“*CO+*CH3O”path,another“*CO+*CHO”coupling path was also detected in photoelectrocatalytic *** selectivity of ethanol was significantly enhanced due to the synthesis of dual-site catalyst and the dual-path coupling path between CO2and HCHO simultaneously driven by light and electricity.

关键词： Photoelectrocatalysis Z-scheme C–C coupling Ethanol

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Boosting hydrocarbon conversion via Cu-doping induced oxygen vacancies on CeO2 in CO2 electroreduction

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Journal of energy Chemistry 2025年第1期100卷 66-76页

作者： Lei Xue Tong Shi Chenhui Han Heng Zhang Fenrong Liu Haorun Li Yan Wang Xiaojun Gu Shanghong Zeng Inner Mongolia key laboratory of Chemistry and Physics of Rare Earth Materials School of Chemistry and Chemical Engineering Inner Mongolia University State key laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences Institute of Catalysis Department of Chemistry Zhejiang University National key laboratory of Baiyunobo Rare Earth Resource Research and Comprehensive utilization Baotou Research Institute of Rare Earths

Conversion of CO2back to hydrocarbons is the most direct way of closing the“carbon cycle”,and its significance is further enlarged if this process is driven by renewable energies such as ***,precisely controlling the product selectivity towards hydrocarbons against the competitive hydrogen evolution remains challenging,especially for Cu-based ***,we report a novel defect engineering strategy,by which Cu-doping-induced oxygen vacancies on CeO2nanorods were effectively created,with adjustable vacancy/Cu *** resulting optimum catalyst shows up to 79% catalytic current density to hydrocarbons （excluding CO）,with 49% faradaic efficiency to *** and density functional theory unveil that the ratio between oxygen vacancy and Cu affects significantly the formation of*CHO and activation of H2O,which leads to the following deep hydrogenation to *** findings may spur new insights for designing and developing more controllable chemical process relevant to CO2utilization.

关键词： Oxygen vacancy Hydrocarbon production Reaction mechanism

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Role of iron ore in enhancing gasification of iron coke:Structural evolution,influence mechanism and kinetic analysis

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International Journal of Minerals,Metallurgy and Materials 2025年第1期32卷 58-69页

作者： Jie Wang Wei Wang Xuheng Chen Junfang Bao Qiuyue Hao Heng Zheng Runsheng Xu School of Chemistry and Materials Science Hubei Engineering UniversityXiaogan 432000China key laboratory for Ferrous Metallurgy and Resources utilization of Ministry of Education Wuhan University of Science and TechnologyWuhan 430081China Institue of Ironmaking Technology Baosteel Central Research InstituteShanghai 201999China State key laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China

The utilization of iron coke provides a green pathway for low-carbon *** uncover the influence mechanism of iron ore on the behavior and kinetics of iron coke gasification,the effect of iron ore on the microstructure of iron coke was ***,a comparative study of the gasification reactions between iron coke and coke was conducted through non-isothermal thermogravimetric *** findings indicate that compared to coke,iron coke exhibits an augmentation in micropores and specific surface area,and the micropores further extend and *** provides more adsorption sites for CO_(2) molecules during the gasification process,resulting in a reduction in the initial gasification temperature of iron *** the heating rate in non-isothermal gasification can enhance the reactivity of iron *** metallic iron reduced from iron ore is embedded in the carbon matrix,reducing the orderliness of the carbon structure,which is primarily responsible for the heightened reactivity of the carbon *** kinetic study indicates that the random pore model can effectively represent the gasification process of iron coke due to its rich pore ***,as the proportion of iron ore increases,the activation energy for the carbon gasification gradually decreases,from 246.2 kJ/mol for coke to 192.5 kJ/mol for iron coke 15wt%.

关键词： low-carbon ironmaking iron coke gasification structural evolution kinetic model

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Oxygen vacancies enriched Ir/WOx catalysts for the directly chem-catalytic conversion of cellulose to ethanol

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Tungsten 2025年第1期 88-99页

作者： Yu-Jing Weng Zhao-Ying Ding Ying-Chao Li Yuan-Feng Wu Yuan-Yang Xu Rui Chen Xiao-Lei Zhao Hai-Yong Wang Da-Lei Zhang Yu-Long Zhang Henan key laboratory of Coal Green Conversion and International Joint Laboratory of Coal Clean Utilization College of Chemistry and Chemical Engineering Henan Polytechnic University key laboratory of Renewable energy Guangzhou Institute of Energy Conversion Chinese Academy of Sciences Liaoning Institute of energy Technology

Tungsten and its oxides are highly versatile catalysts with unique properties that hold great promise for a wide array of applications,including biological pathways and chemical *** chemo-catalysis of cellulose to ethanol presents a promising avenue for ethanol synthesis with the potential for enhanced efficiency compared to conventional methods,offering a sustainable and carbon-neutral alternative to existing petrochemical and biological ***,Ir/WOxcatalysts enriched with oxygen vacancies were meticulously prepared and demonstrated remarkable catalytic performance in converting cellulose to ethanol directly in the presence of tungstic *** catalyst achieved a high ethanol yield of 66.5%under optimal reaction conditions,approaching the theoretical yield limit of traditional ethanol *** results revealed the presence of oxygen defects,Bronsted/Lewis acidity,and Ir nanoclusters on the catalyst surface,working synergistically to facilitate the cascade catalysis of cellulose hydrolysis,sugar retro-aldol condensation reaction,and C2 intermediate hydrodeoxygenation to *** situ Fourier transform infrared spectrometer analysis confirmed the catalyst's ability to enhance the adsorption and activation of ethylene glycol for ethanol *** manipulating subtle structural features,this study offers a fresh perspective on tungsten group catalyst design and underscores the importance of synergistic effects among catalytic sites for the efficient production of ethanol from cellulose.

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Influence factors of methane hydrate formation from ice:Temperature,pressure and SDS surfactant

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Chinese Journal of Chemical Engineering 2019年第2期27卷 405-410页

作者： Weiguo Liu Yanghui Li Xiaohu Xu key laboratory of ocean energy utilization and energy Conservation of Ministry of Education Dalian University of Technology

A series of experiments of forming hydrate from ice powders in different conditions have been carried out with constant volume method to evaluate the influence factors such as pressure, temperature, and SDS surfactant. The change of temperature and pressure were collected as a function of elapsed time, which were used to calculate the gas consumption and hydrate saturation during hydrate formation(pVT method). Based on the experimental results and the analysis, it is concluded that:(1) Both initial pressure and temperature have effect on the hydrate formation and temperature plays a more important role in the process;(2) heating and secondary pressurization will promote the gas hydrate formation and enhance the hydrate saturation as a result. Meanwhile, the promotion of heating seems to be more obvious than that of secondary pressurization;(3) different concentrations of SDS surfactant have clearly influence on the saturation of gas hydrate and there is an optimal concentration to promote the hydrate formation.

关键词： Methane hydrate Ice Heating Secondary pressurization Surfactant

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Dissociation characteristics of methane hydrate using depressurization combined with thermal stimulation

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Chinese Journal of Chemical Engineering 2019年第9期27卷 2089-2098页

作者： Mingjun Yang Zhanquan Ma Yi Gao Lanlan Jiang key laboratory of ocean energy utilization and energy Conservation of Ministry of Education Dalian University of Technology

Methane hydrate is considered as a potential energy source in the future due to its abundant reserves and high energy *** investigate the influence of initial hydrate saturation,production pressure,and the temperature of thermal stimulation on gas production rate and cumulative gas production percentage,we conducted the methane hydrate dissociation experiments using depressurization,thermal stimulation and a combination of two methods in this *** is found that when the gas production pressures are the same,the higher the hydrate initial saturation,the greater change in hydrate reservoir ***,it is easier to appear the phenomenon of icing and hydrate reformation when the hydrate saturation is *** example,the reservoir temperature dropped to below zero in depressurization process when the hydrate saturation was about 37%.However,the same phenomenon didn’t appear as the saturation was about 12%.This may be due to more free gas in the reservoir with hydrate saturated of 37%.We also find that the temperature variation of reservoir can be reduced effectively by combination of depressurization and thermal stimulation *** the average gas production rate is highest with combined method in the *** the pressure of gas production is 2 MPa,compared with depressurization,the average of gas production can increase 54%when the combined method is *** efficiency of gas production is very low when thermal stimulation was used *** the temperature of thermal stimulation is 11℃,the average rate of gas production in the experiment of thermal stimulation is less than 1/3 of that in the experiment of the combined method.

关键词： Methane hydrate Depressurization Thermal stimulation Dissociation characteristics

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