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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 the extrusion parameters on microstructure,texture and room temperature mechanical properties of extruded Mg-2.49Nd-1.82Gd-0.2Zn-0.2Zr alloy

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International Journal of Minerals,Metallurgy and Materials 2025年第1期32卷 136-146页

作者： Chenjin Zhang Guangyu Yang Lei Xiao Zhiyong Kan Jing Guo Qiang Li Wanqi Jie state key laboratory of Solidification Processing Northwestern Polytechnical UniversityXi’an 710072China College of Materials Science and Engineering Fuzhou UniversityFuzhou 350108China College of chemistry and environmental Science Qujing Normal UniversityQujing 655011China

Microstructure,texture,and mechanical properties of the extruded Mg-2.49Nd-1.82Gd-0.2Zn-0.2Zr alloy were investigated at different extrusion temperatures(260 and 320℃),extrusion ratios(10:1,15:1,and 30:1),and extrusion speeds(3 and 6 mm/s).The experimental results exhibited that the grain sizes after extrusion were much finer than that of the homogenized alloy,and the second phase showed streamline distribution along the extrusion direction(ED).With extrusion temperature increased from 260 to 320℃,the microstructure,texture,and mechanical properties of alloys changed *** dynamic recrystallization(DRX)degree and grain sizes enhanced as the extrusion ratio increased from 10:1 to 30:1,and the strength gradually decreased but elongation(EL)*** the extrusion speed increased from 3 to 6 mm/s,the grain sizes and DRX degree increased significantly,and the samples presented the typical-rare-earth(RE)*** alloy extruded at 260℃ with extrusion ratio of 10:1 and extrusion speed of 3 mm/s showed the tensile yield strength(TYS)of 213 MPa and EL of 30.6%.After quantitatively analyzing the contribution of strengthening mechanisms,it was found that the grain boundary strengthening and dislocation strengthening played major roles among strengthening *** results provide some guidelines for enlarging the industrial application of extruded Mg-RE alloy.

关键词： Mg-rare earth alloys extrusion temperature extrusion ratio extrusion speed strengthening mechanisms

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Simultaneous determination of ten taste and odor compounds in drinking water by solid-phase microextraction combined with gas chromatography-mass spectrometry

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Journal of environmental Sciences 2013年第11期25卷 2313-2323页

作者： Xichao Chen Qian Luo Shengguang Yuan Zi Wei Hanwen Song Donghong Wang Zijian Wang state key laboratory of environmental aquatic chemistry Research Center for Eco-Environmental Sciences Chinese Academy of Sciences

Taste and odor （T＆O） problems in drinking water frequently occur because of many compounds present in the water, of which trans-1,10-dimethyl-trans-9-decalol （geosrnin） and 2-methylisoborneol （MIB） are well-known. In this study, a fast and effective method was established for simultaneous determination of 10 T＆O compounds, including geosmin, MIB, 2,4,6-trichloroanisole （TCA）, 2-methylbenzofuran, 2-isopropyl-3-methoxypyrazine （IPMP）, 2-isobutyl-3-methoxypyrazine （IBMP）, cis-3-hexenyl acetate, trans,trans-2,4-heptadienal, trans, cis-2,6-nonadienal, and trans-2-decenal in water samples by headspace solid-phase microextraction （SPME） coupled with gas chromatography-mass spectrometry. An orthogonal array experimental design was used to optimize the effects of SPME fiber, extraction temperature, stirring rate, NaC1 content, extraction time, and desorption time. The limits of detection ranged from 0.1 to 73 ng/L were lower than or close to the odor threshold concentrations （OTCs）. All the 10 T＆O compounds were detected in the 14 water samples including surface water, treatment process water and tap water, taken from a waterworks in Lianyungang City, China. MIB and geosmin were detected in most samples at low concentration. Six T＆O compounds （IPMP, IBMP, trans,cis-2,6-nonadienal, 2-methylbenzofuran, trans-2-decenal, and TCA） were effectively decreased in water treatment process （sedimentation and filtration） that is different from cis-3-hexenyl acetate, MIB and geosmin. It is noted that the TCA concentrations at 15.9-122.3 ng/L and the trans,cis-2,6-nonadienal concentrations at 79.9-190.1 ng/L were over 10 times higher than their OTCs in tap water. The variation of the analytes in the all water samples, especially distribution system indicated that distribution system cannot be ignored as a T＆O compounds source.

关键词： taste and odor compound drinking water SPME-GC,rMS geosmin 2,4,6-trichloroanisole

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Systematic analysis of microfauna indicator values for treatment performance in a full-scale municipalwastewater treatment plant

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Journal of environmental Sciences 2013年第7期25卷 1379-1385页

作者： Bo Hu Rong Qi Min Yang state key laboratory of environmental aquatic chemistry Research Center for Eco-Environmental Sciences Chinese Academy of Sciences

The indicator values of microfauna functional groups and species for treatment performancewere systematically evaluated based on the continuous monitoring of the entire microfauna communities including both protozoa and metazoa over a period of 14 months, in two parallel full-scale municipalwastewater treatment systems in a plant in Beijing, China. A total of 57 species of ciliates, 14 species （units） of amoebae, 14 species （units） of flagellates and4 classes of small metazoawere identified,with Arcella hemisphaerica, Vorticella striata, Vorticella convallaria, Epistylis plicatilis and small flagellates （e.g. Bodo spp.） as thedominant protozoa, and rotifers as thedominant metazoa. The abundance of the sessile ciliateswas correlatedwith the removals of BOD 5 （Pearson＇s r = 0.410, p 〈 0.05） and COD Cr （r = 0.397, p 〈 0.05）while the testate amoebaewas significantly positively related to nitrification （r = 0.523, p 〈 0.01）. At the same time, some other associationswere also identified： the abundances of the large flagellates （r = 0.447, p 〈 0.01）, the metazoa （r = 0.718, p 〈 0.01） and species Aspidisca sulcata （r = 0.337, p 〈 0.05）were positively related to nitrification; the abundance of Aspidisca costatawas correlated to the TN （total nitrogen） removal （r = -0.374, p 〈 0.05 ）; the abundances of the sessile species Carchesium polypinum （r = 0.458, p 〈 0.01） and E. plicatilis （r = 0.377, p 〈 0.05）were correlatedwith the removal of suspended solids.

关键词： protozoan metazoan activated sludge treatment performance bioindicator

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Preparation and evaluation of Zr-β-FeOOH for efficient arsenic removal

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Journal of environmental Sciences 2013年第4期25卷 815-822页

作者： Xiaofei Sun Chun Hu Jiuhui Qu state key laboratory of environmental aquatic chemistry Research Center for Eco-Environmental SciencesChinese Academy of Sciences

A Zr-β-FeOOH adsorbent for both As（Ⅴ） and As（Ⅲ） removal was prepared by a chemical co-precipitation method. Compared with β-FeOOH, the addition of Zr enhanced the adsorption capacities for As（Ⅴ） and As（Ⅲ）, especially As（Ⅲ）. The maximum adsorption capacities for As（Ⅲ） and As（Ⅴ） were 120 and 60 mg/g respectively at pH 7.0, much higher than for many reported adsorbents. The adsorption data accorded with Freundlich isotherms. At neutral pH, for As（Ⅴ）, adsorption equilibrium was approached after 3 hr, while for As（Ⅲ）, adsorption equilibrium was approached after 5 hr. Kinetic data fitted well to the pseudo second-order reaction model. As（Ⅴ） elimination was favored at acidic pH, whereas the adsorption of As（Ⅲ） by Zr-β-FeOOH was found to be effective over a wide pH range of 4-10. Competitive anions hindered the adsorption according to the sequence： phosphate 〉 silicate 〉 bicarbonate 〉 sulfate 〉 nitrate, while Ca2＋ and Mg2＋ increased the removal of As（Ⅲ） and As（Ⅴ） slightly. The high adsorption capability and good performance in other aspects make Zr-β-FeOOH a potentially attractive adsorbent for the removal of both As（Ⅲ） and As（Ⅴ） from water.

关键词： arsenic adsorbent adsorption kinetic Zr-β-FeOOH

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A fishy odor episode in a north China reservoir: Occurrence, origin, and possible odor causing compounds

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Journal of environmental Sciences 2013年第12期25卷 2361-2366页

作者： Yunyun Zhao Jianwei Yu Ming Su Wei An Min Yang state key laboratory of environmental aquatic chemistry Research Center for Eco-Environmental SciencesChinese Academy of Sciences

A significant outbreak of fishy odor occurred in a reservoir located in Inner Mongolia, China, in the winter of 2011, and the odor rating, algal density and concentrations of some potential odorous compounds were monitored over a period of two months. The peak odor rating of the fishy odor was 7 according to flavor profile analysis. Among the dominant algal species （two diatom and one chrysophyte species） observed during the survey, the chrysophyte Dinobryon sp. was the most abundant species, with the peak density recorded at 88,520 cells/mL. Seven potential algal metabolites including heptanal, 2,4-heptadienal, 2,4-decadienal, nonanal, 2-octenal, 2,6- nonadienal and hexanal were detected. The principal component analysis result showed that n-hexanal, n-heptanal and 2,4-decadienal, possibly the metabolites of diatoms, and 2,4-heptadienal, possibly the metabolite of Dinobryon sp., might have contributed to the fishy odor episode. This study demonstrated that the fishy odor episode in this reservoir might be caused by the abnormal growth of chrysophytes and diatoms under the ice-cover.

关键词： fishy odor chrysophyte diatom reservoir drinking water flavor profile analysis

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Preparation and characterization of organic polymer modified composite polyaluminum chloride

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Journal of environmental Sciences 2006年第2期18卷 214-220页

作者： SHI Bao-you TANG Hong-xiao state key laboratory of environmental aquatic chemistry Chinese Academy of Sciences Beijing 100085 China

Compared with traditional aluminum salts, polyaluminum chloride （PACI） has better coagulation-flocculation performance in turbidity removal. However, it is still inferior to organic polymers in terms of bridging function. In order to improve the aggregating property of PACl, different composite PACl flocculants were prepared with various organic polymers. The effect of organic polymer on the distribution or Al（Ⅲ） species in composite flocculants was studied using ^27TAl NMR and Al-ferron complexation methods. The charge neutralization and surface adsorption characteristics of composite flocculants were also investigated. Jar tests were conducted to evaluate the turbidity removal efficacy of organic polymer modified composite flocculants. The study shows that cationic polymer and anionic polymer have significant influences on the coagulation-flocculation behaviors of PACl. Both cationic and anionic polymers can improve the turbidity removal performancc of PACl but the mechanisms arc much different： cationic organic polymer mainly increases the charge neutralization ability, but anionic polymer mainly enhances the bridging function.

关键词： polyaluminum chloride(PACl) organic polymer composite flocculant

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Relationship between heavy metals and dissolved organic matter released from sediment by bioturbation/bioirrigation

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Journal of environmental Sciences 2019年第1期31卷 216-223页

作者： Yi He Bin Men Xiaofang Yang Yaxuan Li Hui Xu Dongsheng Wang state key laboratory of environmental aquatic chemistry Research Centre for Eco-Environmental Science Chinese Academy of Sciences

Organic matter(OM) is an important component of sediment. Bioturbation/bioirrigation can remobilize OM and heavy metals that were previously buried in the sediment. The remobilization of buried organic matter, thallium(Tl), cadmium(Cd), copper(Cu) and zinc(Zn) from sediment was studied in a laboratory experiment with three organisms: tubificid,chironomid larvae and loach. Results showed that bioturbation/bioirrigation promoted the release of dissolved organic matter(DOM) and dissolved Tl, Cd, Cu and Zn, but only dissolved Zn concentrations decreased with exposure time in overlying water. The presence of organisms altered the compositions of DOM released from sediment,considerably increasing the percentage of fulvic acid-like materials(FA) and humic acidlike materials(HA). In addition, bioturbation/bioirrigation accelerated the growth and reproduction of bacteria to enhance the proportion of soluble microbial byproduct-like materials(SMP). The DOM was divided into five regions in the three-dimensional excitation emission matrix(3 D-EEM), and each part had different correlation with the dissolved heavy metal concentrations. Dissolved Cu had the best correlation with each of the DOM compositions, indicating that Cu in the sediment was in the organic-bound ***, the organism type and heavy metal characteristics both played a role in influencing the remobilization of heavy metal.

关键词： Bioturb ation/bioirrigation Heavy metal Sediment DOM

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Spatial and temporal variations of two cyanobacteria in the mesotrophic Miyun reservoir, China

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Journal of environmental Sciences 2014年第2期26卷 289-298页

作者： Ming Su Jianwei Yu Shenling Pan Wei An Min Yang state key laboratory of environmental aquatic chemistry Research Center for Eco-Environmental Sciences Chinese Academy of Sciences

Spatial variations in phytoplankton community within a large mesotrophic reservoir （Miyun reservoir, North China） were investigated in relation to variations in physico-chemical properties, nutrient concentrations, temperature and light conditions over a 5 month period in 2009. The dynamics of phytoplankton community was represented by the dominance of cyanobacteria through summer and fall, following with a short term dominance of chlorophyta in late fall, and a relatively high abundance of diatom in October; on the other hand, maximum phytoplankton biomass was recorded in the north shallow region of Miyun reservoir with a higher nutrients level. Particular attention was paid to the impacts of environmental conditions on the growth of two cyanobacteria genera, the toxin-producing Microcystis and the taste ＆ odor-producing Oscillatoria. Microcystis biomass was in general greatly affected by water temperature and mixing depth/local water depth ratio in this reservoir, while the Oscillatoria biomass in the surface and middle layers was greatly affected by total dissolved phosphorus, and that in the bottom layer was related with the Secchi depth/local water depth ratio. Abundant Oscillatoria biomass was observed only in late September when Microcystis biomass decreased and allowed sufficient light go through.

关键词： phytoplankton community succession Microcystis sp. Oscillatoria sp. mesotrophic reservoir total dissolved phosphorus water transparency mixing process

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Risk assessment of Giardia from a full scale MBR sewage treatment plant caused by membrane integrity failure

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Journal of environmental Sciences 2015年第4期27卷 252-258页

作者： Yu Zhang Zhimin Chen Wei An Shumin Xiao Hongying Yuan Dongqing Zhang Min Yang state key laboratory of environmental aquatic chemistry Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Tianjin key laboratory of aquatic Science and Technology Tianjin Chengjian University

Membrane bioreactors（MBR） are highly efficient at intercepting particles and microbes and have become an important technology for wastewater reclamation. However, many pathogens can accumulate in activated sludge due to the long residence time usually adopted in MBR, and thus may pose health risks when membrane integrity problems *** study presents data from a survey on the occurrence of water-borne Giardia pathogens in reclaimed water from a full-scale wastewater treatment plant with MBR experiencing membrane integrity failure, and assessed the associated risk for green space irrigation. Due to membrane integrity failure, the MBR effluent turbidity varied between 0.23 and 1.90 NTU over a period of eight months. Though this turbidity level still met reclaimed water quality standards（≤ 5 NTU）, Giardia were detected at concentrations of 0.3 to 95 cysts/10 L, with a close correlation between effluent turbidity and Giardia concentration. All β-giardin gene sequences of Giardia in the WWTP influents were genotyped as Assemblages A and B, both of which are known to infect humans. An exponential dose–response model was applied to assess the risk of infection by Giardia. The risk in the MBR effluent with chlorination was9.83 × 10-3, higher than the acceptable annual risk of 1.0 × 10^-4. This study suggested that membrane integrity is very important for keeping a low pathogen level, and multiple barriers are needed to ensure the biological safety of MBR effluent.

关键词： Giardia Reclaimed water Water quality Risk Genotype

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