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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： Activation energy

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A simple guideline to apply excitation-emission matrix spectroscopy(EEMs)for the characterization of dissolved organic matter(DOM)in anoxic marine sediments

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Acta Oceanologica Sinica 2023年第1期42卷 109-119页

作者： Shuchai Gan Verena BHeuer Frauke Schmidt Lars Wörmer Kai-Uwe Hinrichs marum—center for marine environmental sciences University of BremenBremenD-28359Germany

marine sediments represent a major carbon reservoir on *** organic matter(DOM)in pore waters accumulates products and intermediates of carbon cycling in *** application of excitation-emission matrix spectroscopy(EEMs)in the analysis of subseafloor DOM samples is largely unexplored due to the redox-sensitive matrix of anoxic pore ***,this study aims to investigate the interference caused by the matrix on EEMs and propose a guideline to prepare pore water samples from anoxic marine *** parameters determined by fluorescence spectra include 3D-index derived from EEMs after parallel factor analysis(PARAFAC),fluorescence index(FI)(contribution of terrigenous DOM),biological index(BIX)and humification index(HIX)derived from 2D emission ***,we investigated the impacts of extensively-presented ions as typical electron acceptors,which are utilized by anaerobic microbes and stratified in marine sediments:Fe(II),Fe(III),Mn(II)and sulfide in anoxic pore water resulted in biases of fluorescent *** proposed threshold concentrations of these ions when the interference on EEMs *** removal of sulfide from sulfide-rich samples could be achieved by flushing with N_(2)for 2 ***,the tests based on DOM standard were further verified using pristine samples from marine *** was a significant change in the fluorescence spectra of DOM in anoxic sediments from the Rhône *** study demonstrated that the change was caused by oxidation of the matrix rather than the intrinsic alteration of *** was confirmed by extracted DOM via both EEMs analysis and Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR-MS).Slight oxidation of sulfur-containing compounds(e.g.,sulfhydryl)and polyphenol-like compounds ***,a sample preparation sequence is proposed for pore water from anoxic *** method enables measurement with small volumes of the sample(e.g.,50µL in this study)an

关键词： marine subsurface sediment EEMs PARAFAC FT-ICR-MS anaerobic pore water

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Geochemistry of Middle Holocene Sediments from South Yellow Sea: Implications to Provenance and Climate Change

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Journal of Earth Science 2016年第5期27卷 751-762页

作者： Xiaoxia Lii Gerard J. M. Versteegh Jinming Song Xuegang Li Huamao Yuan Ning Li Faculty of marine sciences China University of Geosciences State Key Laboratory of Biogeology and environmental Geology China University of Geosciences Heisenberg Group on marine Kerogen Center for Marine Environmental Sciences (MARUM) Bremen University Institute of Oceanology Chinese Academy of Sciences

From a large number of case studies on terrestrial deposits we know that Late Holocene climate fluctuations have an important impact on the terrestrial environments. However, it is hitherto not clear how the marine sediments can be used to shed light on the environment and climate change of the catchment. To provide such insight, we used the major element, trace element and rare earth element（REE） compositions in the southern Yellow Sea（SYS） sediments to reconstruct the changes in weathering and erosion of their source regions. The sediments originate predominantly from the upper crust of East China and are transported into the basin especially by the Yellow River（Huanghe） and to a lesser extent by the Yangtze River（Changjiang）. The chemical index of alteration（CIA; 53.7–59.7） suggests low chemical weathering of the source rocks since the Middle Holocene. This is consistent with the relatively cool and arid climate in North China after the Holocene Megathermal. Comparison of element ratios, including Al/Ca, K/Ca, Al/Na, K/Na, Rb/Sr, Li/Ba and the CIA shows that we can use the latter as a robust proxy for climate change. The CIA-based mean annual precipitation and mean annual temperature show a series of climate fluctuations in the catchment. A relatively warm and humid Period I（5.3–2.9 cal. ka BP）, a relatively cool and dry Period II（2.9–0.9 cal. ka BP） and an increasingly cool and dry Period III（0.9–0.3 cal. ka BP）. These periods can be linked to climate intervals recognized elsewhere.

关键词： geochemical composition elemental ratio climate change provenance South YellowSea sediment.

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The geobiological formation process of the marine source rocks in the Middle Permian Chihsia Formation of South China

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Science China Earth sciences 2014年第5期57卷 957-964页

作者： LIU XiTing YAN JiaXin XUE WuQiang MA ZhiXin LI Bo Faculty of Earth sciences and State Key Laboratory of Biogeology and environmental Geology China University of Geosciences marum-center for marine environmental sciences University of Bremen Chengdu Institute of Geology and Mineral Resources Guangzhou marine Geological Survey

The Chihsia Formation is one of the four sets of regional marine hydrocarbon source rocks from South *** the past two decades,detailed geochemical and sedimentological studies have been carried out to investigate its origination,which have demonstrated that the high primary productivity plays a primary role in the deposition of sediments enriched in the organic ***,the mechanism of this high productivity and the path of the deposition and burial of the organic matter have always been a *** on the previous studies on the Shangsi Section in Guangyuan City,Sichuan Province,we proposed that the development of the equatorial upwelling due to the sea level rise is responsible for the relatively high productivity in the Chihsia *** sea waters with high nutrient were transported by the sub-surface currents along the *** organic carbon flux was deposited on the deeper shelf,and then decomposed by bacteria,leading to the occurrence of anaerobic *** metabolism of the microorganisms consumed the dissolved oxygen in waters,which was in favor of the preservation of the organic *** suggested geobiological model integrating with paleoclimatology,paleoceanography and geomicrobiology will help us to understand the causes of this particular sedimentary sequence.

关键词： Chihsia Formation source rocks primary productivity paleo-oxygenation facies geobiology South China

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Evolution of the East China Sea sedimentary environment in the past 14 kyr: Insights from tetraethers-based proxies

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Science China Earth sciences 2016年第5期59卷 927-938页

作者： GE HuangMin ZHANG ChuanLun VERSTEEGH Gerard J.M. CHEN LingLing FAN DaiDu DONG Liang LIU JingJing State Key Laboratory of marine Geology Tongji University Hadal Science and Technology Research center (Shanghai Engineering Research center of Hadal Science and Technology) Shanghai Ocean University Heisenberg Group on marine Kerogen Center for Marine Environmental Sciences (MARUM) Bremen University

We reconstruct the environmental evolution of the East China Sea in the past 14 kyr based on glycerol dialkyl glycerol tetraethers(GDGTs) in a sediment core from the subaqueous Yangtze River Delta. Two primary phases are recognized. Phase I(13.8–8 cal kyr BP) reflects a predominantly continental influence, showing distinctly higher concentrations of branched GDGTs(averaged 143 ng/g dry sediment weight, dsw) than isoprenoid GDGTs(averaged 36 ng/g dsw), high BIT index(branched vs. isoprenoid tetraethers) values(>0.78) and a fluctuating GDGT-0/crenarchaeol ratio(R_(0/5), varied from 0.52 to 3.81). Within this interval, temporal increases of terrestrial and marine influence are attributed to Younger Dryas(YD)(ca. 12.9–12.2 cal kyr BP) cold event and melt-water pulse(MWP)-1B(11.5–11.1 cal kyr BP), respectively. The prominent transition from 8 to 7.9 cal kyr BP shows a sharp decrease in BIT index value(<0.4) and increase in crenarchaeol, which marks the beginning of phase II. Afterwards, the proxies remain relatively constant, which indicates that phase II(7.9 cal kyr BP-present) is a shelf sedimentary environment with high stand of sea level. Overall, the BIT index in our record serves as a good marker for terrestrial influence at the site, and likely reflects the flooding history of the region. The TEX_(86)(Tetra Ether Index of tetraethers consisting of 86 carbons) proxy is not applicable in phase I because of an excess terrestrial influence; but it seems to be valid for revealing the annual SST in phase II(21.6±0.9°C, n=49). In contrast, the MBT'/CBT(Methylation of Branched Tetraethers and Cyclization of Branched Tetraethers) proxy appears to faithfully record the annual mean air temperature(MAT)(14.3±0.63°C, n=68) and presents an integrated signal over the middle and lower Yangtze River drainage basin.

关键词： GDGTs Proxies Sedimentary environment evolution Holocene East China Sea

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Arsenic and sulfur nanoparticle synthesis mimicking environmental conditions of submarine shallow-water hydrothermal vents

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Journal of environmental sciences 2022年第1期34卷 301-312页

作者： Vicente Durán-Toro Kurosch Rezwan Solveig I.Bühring Michael Maas marum–center for marine environmental sciences University of BremenBremen 28359Germany Advanced Ceramics University of BremenBremen 28359Germany MAPEX-center for Materials and Processes University of BremenBremen 28359Germany

Arsenic and sulfur mineralization is a natural phenomenon occurring in hydrothermal systems where parameters like temperature and organic matter(OM)can influence the mobilization of the toxic metalloid in marine *** the present study we analyze the influence of temperature and OM(particularly sulfur-containing additives)on As and S precipitation based on the recent discovery of As-rich nanoparticles in the hydrothermal system near the coast of the Greek island *** this end,we experimentally recreate the formation of amorphous colloidal particles rich in As and S via acidification(pH 3–4)of aqueous precursors at various *** higher temperatures,we observe the formation of monodisperse particles within the first 24 h of the experiment,generating colloidal particles with diameters close to 160 *** S:As ratio and particle size of the synthetized particles closely correlates with values for As_(x)S_(y)particles detected in the hydrothermal system off ***,organic sulfur containing additives(cysteine and glutathione,GSH)are a key factor in the process of nucleation and growth of amorphous colloidal As_(x)S_(y)particles and,together with the temperature gradient present in shallow hydrothermal vents,dictate the stabilization of As-bearing nanomaterials in the *** on these findings,we present a simple model that summarizes our new insights into the formation and mobility of colloidal As in aquatic *** this context,amorphous As_(x)S_(y)particles can present harmful effects to micro-and macro-biota not foreseen in bulk As material.

关键词： Biomineralization Milos Hydrothermal vent Arsenic Sulfur Nanoparticles Ecotoxicology

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Evaluating the Mechanism of Tropical Expansion Using Idealized Numerical Experiments

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Ocean-Land-Atmosphere Research 2023年第1期2卷 44-56页

作者： Hu Yang Gerrit Lohmann Xiaoxu Shi Juliane Müller Alfred Wegener Institute Helmholtz Centre for Polar and Marine ResearchBremerhavenGermany University of Bremen Center for Marine Environmental SciencesMARUMBremenGermany

A wide range of evidence reveals that the tropical belt is *** mechanisms have been proposed to contribute to this expansion,some of which even contradict each *** study of Yang et *** that the poleward advancing mid-latitude meridional temperature gradient(MTG),originating from enhanced subtropical ocean warming,plays a leading role in driving tropical ***,the abrupt4xCO_(2) experiment indicates that tropical expansion occurs at a faster rate than is indicated by changes related to ocean temperature *** idealized amip4K experiment illustrates that without introducing any ocean warming pattern,uniform ocean surface warming also drives tropical *** results based on these idealized experiments seem to contradict the hypothesis proposed by Yang et *** this study,we revisit these 2 experiments and show that both experiments actually support the hypothesis that MTG migration is driving tropical *** specifically,in the abrupt4xCO_(2) experiment,although the rate of ocean warming is relatively slow,the poleward shift of the MTG is as rapid as tropical *** the amip4K experiment,although ocean surface warming is uniform,the heating effect of the ocean on the atmosphere is nonuniform because of the nonlinear relationship between temperature,evaporation,and thermal *** nonuniform oceanic heating to the atmosphere introduces a poleward shift of the MTG within the upper troposphere and drives a shift in the jet *** conducting an additional idealized experiment in which tropical expansion occurs under both a migrating MTG and a cooling climate,we argue that the migration of the MTG,rather than global warming,is the key mechanism in driving tropical expansion.

关键词： warming ocean tropical

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Linkage Between Winter Temperatures in the Yellow Sea and Atmospheric Circulation Indices

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Journal of Ocean University of China 2019年第2期18卷 261-270页

作者： YUAN Chengyi WEI Hao LUO Xiaofan KUANG Xiaodi College of marine and environmental sciences Tianjin University of Science and Technology School of marine Science and Technology Tianjin University National marine environmental Forecasting center

This study investigated the linkage between winter temperature in the Yellow Sea(YS), China, and atmospheric indices and established this linkage through statistical models. The water temperature was obtained through hindcast simulation using a global–regional nested ocean model for the period of 1958–2007. The interannual variations of the simulated temperature were validated using satellite and in-situ observations. In the YS, the winter sea surface temperature(SST) had obvious interannual variations, with the maximum SST exceeding 2℃, and a significant shift from the cold to warm phase during 1988–1989. Based on the mechanism study, statistical models for the variations of water temperature in the YS were established using suitable atmospheric indices as predictors. For the northern YS(NYS) and the coastal region of the southern YS(SYS), statistical models of SST were established using linear regression based on the December–January–February mean Arctic oscillation index(AOI), representing the dominant large-scale atmospheric variability in boreal winter. For the YS warm current(YSWC) region, statistical models were established using both the AOI and the first principal component of the local wind stress curl(PC1-Curl), derived from the empirical orthogonal functions analysis. The PC1-Curl represents the influence of the local wind stress curl on the west-to-east shifts of the YSWC pathway. The applications proved that the models presented in this study have the ability to estimate winter temperatures in the YS within the recent years.

关键词： water temperature statistical model interannual variations atmospheric variability empirical orthogonal function analysis

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Aerobic anoxygenic phototrophic bacteria and their roles in marine ecosystems

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Chinese Science Bulletin 2003年第11期48卷 1064-1068页

作者： JIAO Nianzhi Michael E. Sieracki ZHANG Yao DU Hailian Key Lab for marine environmental sciences of Ministry of Education Center for Marine Environmental Sciences Xiamen UniversityBigelow Laboratory for Ocean SciencesKey Lab for Marine Environmental Sciences of Ministry of Education Center for Marine Environmental Sciences Xiamen UniversityKey Lab for Marine Environmental Sciences of Ministry of Education Center for Marine Environmental Sciences Xiamen University Xiamen 361005 ChinaME 04575 USAXiamen 361005 ChinaXiamen 361005 China

Aerobic anoxygenic phototrophic bacteria (AAPB) are characterized by the following physiological and ecological features. A mother AAPB cell can unusually divide into 3 daughter cells and looks like a 揧?during the division. AAPB cells sometimes adhere together forming a free-floating population. Most of the known AAPB species are obligately aerobic. Bacteriochlorophyll a (BChl a) is the only photosynthetic pigment in AAPB, and the number of BChl a molecules in an AAPB cell is much less than that in an anaerobic phototrophic bacterial cell, while the accessorial pigments carotenoids in AAPB are abundant in concentration and diverse in species. In addition to the common magnesium containing BChl a, a zinc-containing BChla was also seen in AAPB. AAPB have light harvesting complexⅠbut usually lack light harvesting complexⅡ. Although AAPB featur in photosynthesis, their growth is not necessarily light- dependent. There is a mechanism controlling the photosynthesis approach. AAPB are widely distributed in marine environments especially in oligotrophic oceans accounting for a substantial portion of the total biomass and playing a unique role in the cycle of carbon and other biogenic elements. Besides the contribution to primary production, AAPB also have great potentials in bioremediation of polluted environments. Studies on AAPB would be of great value in understanding the evolution of photosynthesis and the structure and function of marine ecosystems.

关键词：光合作用海洋生态系统 AAPB 需氧光养细菌细菌叶绿素母细胞子细胞色素类胡萝卜素光养菌分类

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Application of an integrated methodology for eutrophication assessment:a case study in the Bohai Sea

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Chinese Journal of Oceanology and Limnology 2013年第5期31卷 1064-1078页

作者：吴在兴俞志明宋秀贤袁涌铨曹西华梁玉波 Key Laboratory of marine Ecology and environmental Science Institute of OceanologyChinese Academy of Sciences University of Chinese Academy of sciences National marine environmental Monitoring center

An integrated methodology for eutrophication assessment,which integrates both water quality indicators(causative factors) and ecological response indicators(effect factors),is *** is then applied to rank the eutrophication status of the years 2007 and 2008 in the southwest Bohai *** assessment model identified that north Bohai Bay and west Laizhou Bay were the two areas with the most serious eutrophication problems in the southwest Bohai *** addition,compared to that in the west Laizhou Bay,the eutrophication conditions in the north Bohai Bay was more serious in both *** problems such as harmful algal blooms(HABs) and low dissolved oxygen(DO) events in north Bohai Bay were *** integrated method outmatched the currently used Chinese nutrient index method by definitely identifying areas with the most serious eutrophication problems,while the nutrient index method gave ambiguous results between the two *** of both causative factors and effect factors,combining concentration,spatial coverage and frequency of indicators,as well as use of multi-season monitoring datasets in the methodology result in a more accurate,representative and useful assessment.

关键词： eutrophication assessment Bohai Sea water quality ecological response

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