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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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Effects of carbon content on the microstructure and tensile properties of a low-density steel

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International Journal of Minerals,Metallurgy and Materials 2025年第2期32卷 391-401页

作者： Yongxuan Shang Mingyu Fan Shuyong Jiang Zhongwu Zhang key laboratory of Superlight Materials and Surface Technology Ministry of EducationCollege of Materials Science and Chemical EngineeringHarbin Engineering UniversityHarbin 150001China state key laboratory of Metal Material for marine Equipment and Application Iron&Steel Research Institute of Ansteel Group CorporationAnshan 114009China

Carbon can change the phase components of low-density steels and influence the mechanical *** this study,a new method to control the carbon content and avoid the formation ofδ-ferrite by decarburization treatment was *** microstructural changes and mechanical characteristics with carbon content induced by decarburization were systematically ***-Jaoul(C-J)analysis was employed to examine the work hardening characteristics during the tensile *** decarburization by heat treatments,the carbon content within the austenite phase decreased,while Mn and Al were almost unchanged;this made the steel with full austenite transform into the austenite and ferrite dual ***,(Ti,V)C carbides existed in both matrix phase and the mole fraction almost the *** addition,the formation of other carbides *** loss induced a decrease in strength due to the weakening of the carbon solid *** the steel with the single austinite,the deformation mode of austenite was the dislocation planar glide,resulting in the formation of *** the dual-phase steel,the deformation occurred by the dislocation planar glide of austenite first,with the increase in strain,the cross slip of ferrite took place,forming dislocation cells in *** the late stage of deformation,the work hardening of austinite increased rapidly,while that of ferrite increased slightly.

关键词： low-density steels carbon content decarburization strengthening mechanisms work hardening behavior

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Temporal and spatial evolution of a deep-reaching anticyclonic eddy in the South China Sea

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Science China Earth Sciences 2019年第6期62卷 1002-1023页

作者： Meng WANG Yanwei ZHANG Zhifei LIU Yulong ZHAO Jianru LI state key laboratory of marine geology Tongji University

The temporal and spatial evolution of a deep-reaching anticyclonic eddy(AE) is studied using a combination of satellite measurements, moored observations and ocean model reanalysis data in the South China Sea(SCS). Three evolutionary stages in eddy's lifecycle are identified from changes in eddy dynamical characteristics estimated from satellite altimetry: birth(22 days), growth(64 days), and decay(47 days). Similar patterns are also distinguished from dynamic signals in ***, flows reversal and upwelling of cold water below 1500 m were captured by the in-situ records when this energetic,highly nonlinear and long-lived(over 19 weeks) AE passed by our mooring position. Its detailed vertical structure is examined through temperature anomalies, vertical shear of horizontal velocities, and horizontal streamlines estimated from ocean model reanalysis data. Results from the model reveal a mesoscale AE with first-mode baroclinic structure: a bowl-shaped anticyclonic flow in the upper ocean connected to a slant-cylinder cyclonic flow at depth, with a transition layer at depths between 400 and 700 m. It is in good agreement with moored observations but showing a shallower transition depth, suggesting a slight deficiency in the model due to limited deep-sea observations. Last, we estimate eddy heat transport at different depths and stages along the AE's path based on the model data. The result reveals that pronounced heat fluxes occur during growth stage(depths 700–1500 m).Dynamical characteristics suggest that the vertical structure and temporal evolution of the eddy play significant roles in basinscale movement and heat transferring. Considering that mesoscale eddies are ubiquitous in the SCS, our results support a recently-proposed mechanism, whereby upper ocean flows produce changes in the deep-sea circulation, potentially influencing boundary l

关键词： Deep-reaching mesoscale eddy Evolution HYCOM The South China Sea

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Exploring the deep South China Sea: Retrospects and prospects

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Science China Earth Sciences 2019年第10期62卷 1473-1488页

作者： Pinxian WANG Zhimin JIAN state key laboratory of marine geology Tongji University

Rapid developments of deep-sea researches in China over the past 20 years have promoted the South China Sea(SCS) into the international deep-sea frontiers. The 'three deep technologies', namely scientific drilling, long-term seafloor observation and deep submersible vehicles implemented successively in SCS studies helped to achieve a number of scientific breakthroughs. Over the 20 years, five international ocean drilling expeditions to the SCS recovered nearly 10 km of sediment cores from sites at 3–4 km water depths, and drilling into the magmatic basement at 6 sites shed light on the genesis of the SCS basin. Coupled with other deep-sea short core sediments from the SCS, these records demonstrate evidence that water and carbon cycling in the low latitude regions can directly respond to the orbital forcing, and subsequently nurture a new concept of lowlatitude forcing of climate changes, which challenges the classical wisdom of the overwhelming role played by the Arctic icesheet in climate changes. The exploration in the continent-ocean transition zone also reveals a number of specific features that characterize the SCS as a marginal basin formed at the subduction zone in the Western Pacific. The features include active magmatism and rapid rupture of lithosphere through the basin formation process, and imply that 'the SCS is not a mini-Atlantic'as they can be distinguished as 'plate-edge rifting' and 'inner-plate rifting' respectively, thus challenging the universality of the Atlantic model for passive margins. Many more discoveries can be assembled from long-term mooring observations and deep diving cruises in the deep SCS, such as the cyclonic nature of the deep-water circulation, deep-water sediment transport by contour currents and turbidites, manganese nodules, extinct hydrothermal vents, and cold-water coral forests. In addition,prominent progress achieved in microbiology and biogeochemistry includes the microbial carbon pump and the coupling of carbon and ni

关键词： Deep sea Marginal sea Ocean drilling Climate change Seafloor observation South China Sea

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Seasonal variability of tides in the deep northern South China Sea

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Science China Earth Sciences 2019年第4期62卷 671-683页

作者： Jiuqiang ZHAO Yanwei ZHANG Zhifei LIU Yulong ZHAO Meng WANG state key laboratory of marine geology Tongji University

Tides are the major energy source for ocean mixing, regulating the variation of oceanic circulation and sediment transport in the deep sea. Here twenty months of high-resolution current profiles, which were observed via a mooring system at a water depth of 2100 m in the northern South China Sea(SCS), are used to investigate seasonal variability in deep-sea *** analysis shows that tides in this region are dominated by diurnal tide, and both diurnal and semidiurnal tide are vertical mode-1 dominant. Baroclinic diurnal tidal current exhibits pronounced seasonal variability, showing its kinetic energy was the strongest in summer, and the maximum depth-averaged value was up to 86.7 cm^2 s^(-2), which was about 1.5 times of that in winter and twice that in spring and autumn. In contrast, baroclinic semidiurnal tide displays no evident seasonal variability. Such seasonal variability in baroclinic tide was mainly modulated by the barotropic forcing from the Luzon Strait. On the other hand,two anticyclonic eddies and one cyclonic eddy, which originated off southwestern Taiwan in winter, crossed the mooring *** cyclonic eddy had weak impact on current velocity in the deep sea, but the two deep-reaching anticyclonic eddies enhanced the current velocity through the full-water column by inducing strong subinertial flows. Consequently, the kinetic energy of tides was strengthened and the incoherent variance of baroclinic diurnal tide increased in winter, which contributed ～85% of the variability in diurnal tide. Meanwhile, the velocity of baroclinic diurnal tide was reduced in winter, which was attributed to the weakened stratification induced by the passage of anticyclonic eddies in the deep sea. The seasonal variability of tides in the deep northern SCS can provide a dynamic mechanism for interpreting sediment transport processes in the deep sea on different time scales.

关键词： Tides Seasonal variability Subinertial current Mesoscale eddy Deep northern South China Sea

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Quantifying the sources of dissolved inorganic carbon within the sulfate-methane transition zone in nearshore sediments of Qi'ao Island, Pearl River Estuary, Southern China

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Science China Earth Sciences 2016年第10期59卷 1959-1970页

作者： WU ZiJun ZHOU HuaiYang REN DeZhang GAO Hang LI JiangTao state key laboratory of marine geology Tongji University

The significance of the various biogeochemical pathways that drive carbon cycling and the relative fractions of dissolved inorganic carbon(DIC) produced by these reactions within the sulfate-methane transition zone(SMTZ) are still being debated. Unraveling these processes is important to our understanding of the benthic DIC sources and their contributions to the global carbon cycle. Here, we measure pore water geochemistry(chlorine, sulfate, methane, Ca^(2+), Mg^(2+), DIC and δ^(13)C-DIC) as well as solid geochemistry(sedimentary organic carbon(SOC) and δ^(13)C of SOC) in nearshore sediments from Qi'ao Island in the Pearl River Estuary of the Southern China Sea. Our analysis indicates that SOC originates from the mixing of carbon from terrestrial and marine sources, and that terrestrial materials dominate the net loss of SOC during the degradation of organic matter, especially at sites located near the river outlets. Sulfate reduction via SOC degradation is not appreciable in the upper sediment layer due to conservative mixing-dilution by freshwater. However, below this layer, the anaerobic oxidation of methane(AOM) and methanogenesis occur. Within the SMTZ, the δ^(13)C mass balance shows that the proportions of DIC derived from organoclastic SO_4^(2-) reduction(OSR) and AOM are 50.3% to 66.7% and 0.1% to 17.9%, respectively, whereas methanogenesis contributes 17.0% to 43.9%. This study reveals that the upward diffusion of DIC from ongoing methanogenesis significantly influences carbon cycling within the SMTZ in these estuarine sediments. As a result, we suggest that the plots of the ratio of change in sulfate to change in DIC in pore water should be used with caution when discriminating between sulfate reduction pathways in methane-rich sediments.

关键词： Dissolved inorganic carbon Sulfate reduction Methane Carbon isotopes Estuaries

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Distinct distribution revealing multiple bacterial sources for 1-Omonoalkyl glycerol ethers in terrestrial and lake environments

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Science China Earth Sciences 2015年第6期58卷 1005-1017页

作者： YANG Huan ZHENG FengFeng XIAO WenJie XIE ShuCheng state key laboratory of Biogeology and Environmental geology China University of Geosciences state key laboratory of marine geology Tongji University

The 1-O-monoalkyl glycerol ethers （MAGEs） were initially viewed as the biomarkers for sulfate-reducing bacteria （SRB） me- diating anaerobic oxidation of methane in the marine environments. However, limited information is known about their distri- bution in terrestrial and other aquatic settings including soils, fresh water lakes, and cave sediments, which may obscure our understanding of their biological sources. Here we found that MAGEs were ubiquitous but differed obviously in distributional pattern among those environments. The surface soils are dominated generally by iC15：0-MAGE, followed by nCI6：o-MAGE whereas the lake sediments show the opposite, resulting in significantly higher iC15：0/nC16：0 ratios in soils than in lake sedi- ments. The cave deposits are characterized by considerably higher proportions of branched MAGEs than the former two envi- ronments. The logarithm of iC15：0/aC15：0 ratio shows a significant negative correlation with soil pH, likely reflecting an adapta- tion of microbial cell membrane to change in the ambient proton concentration. The MAGE profiles in cultured bacteria cannot fully explain the MAGE distribution in all the samples analyzed. Therefore, MAGEs in soil, lake sediments, and cave deposits likely have additional biological source（s） other than SRB and cultured MAGE-producing bacteria. The difference in MAGE pattern among environments is likely to be attributed to change in microbial communities.

关键词： 1-O-monoalkyl glycerol ethers soil lake sediments cave deposits biological sources

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Modelling of low-temperature exhumation rate in Dabie Mountain based on (U-Th)/He and fission-track thermochronological data

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Science China Earth Sciences 2006年第10期49卷 1009-1019页

作者： DING Ruxin ZHOU Zuyi XU Changhai LIU Yuzhu CHENG Hao XU Fei state key laboratory of marine geology Tongji UniversityShanghai 200092China State Key Laboratory of Marine GeologyTongji UniversityShanghai 200092China State Key Laboratory of Marine GeologyTongji UniversityShanghai 200092China State Key Laboratory of Marine GeologyTongji UniversityShanghai 200092China State Key Laboratory of Marine GeologyTongji UniversityShanghai 200092China State Key Laboratory of Marine GeologyTongji UniversityShanghai 200092China

While the high-temperature exhumation process in the Dabie Mountain has been well documented, the low-temperature exhumation of this area since Cretaceous, especially since Late Cretaceous, is relatively less studied. Low-temperature thermochronology provides one of the important approaches to solve this problem. Based on the data of fission track and (U-Th)/He analysis of apaptites and zircons from the granitoid and metamorphic rocks in the Dabie Mountain, this paper applies Mancktelow’s and Braun’s methods to estimating the exhumation rates and to drawing the regional differential exhumation pattern since Cretaceous, especially since Late Cretaceous by taking into consideration factors such as heat transport, heat advection, topography and heat production, which could influence geothermal field in the shallow crust. Since Cretaceous, the exhumation rate (0.08-0.10 km/Ma) in the region around Tiantangzhai and in the south of Tanlu fault zone is larger than the rate (0.04-0.07 km/Ma) in other areas of the Dabie Mountain. The regional differential exhumation pattern might be related to the push-up effect caused by differential strike-slip movement along NNE-trending faults.

关键词： Dabie Mountain, fission track, (U-Th)/He, modelling, exhumation.

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Coherent variations of the obliquity components in global ice volume and ocean carbon reservoir over the past 5 Ma

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Science China Earth Sciences 2013年第12期56卷 2160-2172页

作者： TIAN Jun state key laboratory of marine geology Tongji University

The Milankovid theory stresses that the summer insolation in the high northern latitudes that is dominated by the precession cycle controls the glacial/interglacial cycles in global climate change. If the climate system responds linearly to the external insolation forcing, the precession cycle of 23 or 19 ka should dominate the variations in the climatic proxy records. I per- formed spectral and evolutive cross spectral analyses on the high resolution benthic ~80 and oa3C records from the South China Sea and the North Atlantic, the proxies of global ice volume and ocean carbon reservoir respectively. I found that the obliquity instead of the eccentricity or the precession is the most marked cycle in the global ice volume and ocean carbon res- ervoir variations over the past 5 Ma. The analysis further reveals that only at the obliquity band instead of the eccentricity or the precession band does the global ice volume and ocean carbon reservoir display consistently high coherency and stable phase relationship over the past 5 Ma. The consistently positive or near-zero phases of the benthic -o^SO relative to the benthic ff3C at the obliquity band suggest that the global carbon cycle is involved in the polar ice sheet growth as an important internal feedback, not a determinative driving factor. The obliquity instead of the precession or the eccentricity takes the dominant role of driving the global climate change during the Pliocene and Pleistocene.

关键词： global ice volume ocean carbon reservoir obliquity 5 Ma

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Paleo-fluvial sedimentation on the outer shelf of the East China Sea during the last glacial maximum

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Chinese Journal of Oceanology and Limnology 2013年第4期31卷 886-894页

作者：王中波杨守业张志珣蓝先洪顾兆峰张训华 state key laboratory of marine geology Tongji University The key laboratory of marine Hydrocarbon Resources and Environmental geology Ministry of Land and ResourcesQingdao Institute of Marine Geology

Evidence from lithology, foraminiferal assemblages, and high-resolution X-ray fluorescence scanning data of core SFK-1 indicates tidally influenced paleo-fluvial sedimentation during the last glacial maximum (LGM) on the outer shelf of the East China Sea. The paleo-fluvial deposits consist of river channel facies and estuarine incised-valley-filling facies. Different reflections on the seismic profile across core SFK-1 suggest that the river channels shifted and overlapped. River channel deposition formed early in the LGM when sea level fell and the estuary extended to the outer shelf. Channel sediments are yellowish- brown in color and rich in foraminifera and shell fragments owing to the strong tidal influence. Following the LGM, the paleo-river mouth retreated and regressive deposition of estuarine and incised-valley-filling facies with an erosion base occurred. The river channel facies and estuarine incised-valley-filling facies have clearly different sedimentary characteristics and provenances. The depositional environment of the paleo-river system on the wide shelf was reconstructed from the foraminiferal assemblages, CaCO3 content and Ca/Ti ratio. The main results of this study provide further substantial constraints on the recognition of late Quaternary stratigraphy and land-sea interactions on the ECS shelf.

关键词： outer shelf East China Sea LGM (last glacial maximum) paleo-river channel fluvial deposition paleoenvironment

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