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Strategic comparison of membrane-assisted and membrane-less water electrolyzers and their potential application in direct seawater splitting(DSS)

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Green Energy & Environment 2023年第4期8卷 989-1005页

作者： Abdul Malek Xu lu Paul R.Shearing dan j.l.brett Guanjie He Clean Combustion Research Center(CCRC) Physical Science and Engineering Division(PSE)King Abdullah University of Science and Technology(KAUST)Thuwal 23955-6900Kingdom of Saudi Arabia KAUST Solar Center(KSC) Physical Science and Engineering Division(PSE)King Abdullah University of Science and Technology(KAUST)Thuwal 23955-6900Kingdom of Saudi Arabia School of Engineering and Materials Science Queen Mary University of LondonMile End RoadLondon E14NSUK Department of Chemical Engineering University College London(UCL)Gower StLondon WC1E 6BTUnited Kingdom

Electrocatalytic splitting of water by means of renewable energy as the electricity supply is one of the most promising methods for storing green renewable energy as hydrogen. Although two-thirds of the earth’s surface is covered with water, there is inadequacy of freshwater in most parts of the world. Hence, splitting seawater instead of freshwater could be a truly sustainable alternative. However, direct seawater splitting faces challenges because of the complex composition of seawater. The composition, and hence, the local chemistry of seawater may vary depending on its origin, and in most cases, tracking of the side reactions and standardizing and customizing the catalytic process will be an extra challenge. The corrosion of catalysts and competitive side reactions due to the presence of various inorganic and organic pollutants create challenges for developing stable electro-catalysts. Hence, seawater splitting generally involves a two-step process, i.e., purification of seawater using reverse osmosis and then subsequent fresh water splitting. However, this demands two separate chambers and larger space, and increases complexity of the reactor design. Recently, there have been efforts to directly split seawater without the reverse osmosis step. Herein, we represent the most recent innovative approaches to avoid the two-step process, and compare the potential application of membrane-assisted and membrane-less electrolyzers in direct seawater splitting(DSS). We particularly discuss the device engineering, and propose a novel electrolyzer design strategies for concentration gradient based membrane-less microfluidic electrolyzer.

关键词： Electrocatalytic seawater splitting Direct seawater splitting Osmosis Concentration cells Membrane-less electrolyzer Microfluidic electrolyzer

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Characteristics of a gold-doped electrode for application in high-performance lithium-sulfur battery

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journal of Energy Chemistry 2022年第1期31卷 116-128,I0004页

作者： Vittorio Marangon daniele Di lecce dan j.l.brett Paul R.Shearing jusef Hassoun University of Ferrara Department of Chemical and Pharmaceutical SciencesVia Fossato di Mortara 17Ferrara44121Italy Electrochemical Innovation lab Department of Chemical EngineeringUCLLondon WC1E 7JEUnited Kingdom The Faraday Institution Quad OneBecquerel AveHarwell CampusDidcot OX11 ORAUnited Kingdom National Interuniversity Consortium of Materials Science and Technology(INSTM) University of Ferrara Research UnitUniversity of FerraraVia Fossato di Mortara17Ferrara 44121Italy

Bulk sulfur incorporating 3 wt% gold nano-powder is investigated as possible candidate to maximize the fraction of active material in the li-S battery *** material is prepared via simple mixing of gold with molten sulfur at 120℃,quenching at room temperature,and *** comprehensive study reports relevant electrochemical data,advanced X-ray computed tomography(CT)imaging of the positive and negative electrodes,and a thorough structural and morphological characterization of the S:Au 97:3 w/w *** cathode exhibits high rate capability within the range from C/10 to 1C,a maximum capacity above 1300 mAh gs^(-1),and capacity retention between 85%and 91%after 100 cycles at 1C and C/3 *** novel formulation enables a sulfur fraction in the composite cathode film as high as 78 wt%,an active material loading of 5.7 mg cm^(-2),and an electrolyte/sulfur(E/S)ratio of 5μl mg^(-1),which lead to a maximum areal capacity of 5.4 mAh cm^(-2).X-ray CT at the micro-and nanoscale reveals the microstructural features of the positive electrode that favor fast conversion kinetics in the *** analysis of sulfur distribution in the porous cathode displays that electrodeposition during the initial cycle may trigger an activation process in the cell leading to improved ***,the tomography study reveals the characteristics of the lithium anode and the cell separator upon a galvanostatic test prolonged over 300 cycles at a 2C rate.

关键词： lithium-sulfur battery Sulfur loading Electrolyte/sulfur ratio Gold nanoparticles X-ray tomography

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Structure-guided Capacitance Relationships in Oxidized Graphene Porous Materials Based Supercapacitors

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Energy & Environmental Materials 2023年第4期6卷 58-69页

作者： Srinivas Gadipelli Hanieh Akbari juntao li Christopher A.Howard Hong Zhang Paul R.Shearing dan j.l.brett College of Physics Sichuan UniversityChengdu 610064China Electrochemical Innovation lab Department of Chemical EngineeringUniversity College LondonLondonWC1E 7JEUK Department of Physics and Astronomy University College LondonLondonWC1E 6BTUK

Supercapacitors formed from porous carbon and graphene-oxide(GO)materials are usually dominated by either electric double-layer capacitance,pseudo-capacitance,or *** to these combined features,reduced GO materials have been shown to offer superior capacitance over typical nanoporous carbon materials;however,there is a significant variation in reported values,ranging between 25 and 350 F g^(−1).This undermines the structure(e.g.,oxygen functionality and/or surface area)-performance relationships for optimization of cost and scalable *** work demonstrates important structure-controlled charge storage *** this,a series of exfoliated graphene(EG)derivatives are produced via thermal-shock exfoliation of GO precursors and following controlled graphitization of EG(GEG)generates materials with varied amounts of porosity,redox-active oxygen groups and graphitic *** results show significantly varied capacitance values between 30 and 250 F g^(−1)at 1.0 A g^(−1)in GEG structures;this suggests that for a given specific surface area the redox-active and hydrophilic oxygen content can boost the capacitance to 250–300%higher compared to typical mesoporous carbon *** with identical oxygen functionality show a surface area governed *** allows to establish direct structure-performance relationships between 1)redox-active oxygen functional concentration and capacitance and 2)surface area and capacitance.

关键词： electric double-layer capacitance graphene-oxide pseudocapacitance structure-performance relationships supercapacitors

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Realizing optimal hydrogen evolution reaction properties via tuning phosphorous and transition metal interactions

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Green Energy & Environment 2020年第4期5卷 506-512页

作者： Haishun jiang Siyu Zhao Wenyao li Tobias P.Neville Isil Akpinar Paul R.Shearing dan j.l.brett Guanjie He School of Materials Engineering Shanghai University of Engineering ScienceShanghai201620China Electrochemical Innovation lab Department of Chemical EngineeringUniversity College LondonLondonWC1E 7JEUnited Kingdom School of Chemistry University of LincolnJoseph Banks LaboratoriesGreen LaneLincolnLN67DLUnited Kingdom Faculty of Engineering Environmental EngineeringAksaray UniversityAksaray68100Turkey

Hydrogen is one of the most attractive renewables for future energy application,therefore it is vital to develop cost-effective and highlyefficient electrocatalysts for the hydrogen evolution reaction(HER)to promote the generation of hydrogen from mild *** this work,Co–Mo phosphide nanosheets with the adjustable ratio of Co and Mo were fabricated on carbon cloth by a facile hydrothermal-annealing *** to the unique nanostructures,abundant active surfaces and small resistance were *** electrocatalytic performances are obtained,such as the small overpotential of^67.3 mV to realize a current density of 10 mA cm^(-2) and a Tafel slope of 69.9 mV dec^(-1).Rapid recovery of the current response under multistep chronoamperometry is realized and excellent stability retained after the CV test for 2000 *** change of electronic states of different elements was carefully studied which suggested the optimal electrochemical performance can be realized by tuning phosphorous and metal interactions.

关键词： Co-Mo Phosphide Nanosheets Hydrogen evolution reaction Metal-phosphorous interactions

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An adaptive fuel cell hybrid vehicle propulsion sizing model

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iEnergy 2024年第1期3卷 59-72页

作者： jia Di Yang Paul R.Shearing jason Millichamp Theo Suter dan j.l.brett james B.Robinson Electrochemical Innovation lab Department of Chemical EngineeringUniversity College LondonLondon WC1E 7JEUK Advanced Propulsion lab MarshgateUniversity College LondonLondon E202AEUK ZERO Institute Holywell HouseOsney MeadUniversity of OxfordOxfordOX20ES The Faraday Institution Quad OneBecquerel AvenueHarwell Science and Innovation CampusDidcot OX110RAUK

As we enter the age of electrochemical propulsion,there is an increasing tendency to discuss the viability or otherwise of different electrochemical propulsion systems in zero-sum *** discussions are often grounded in a specific use case;however,given the need to electrify the wider transport sector it is evident that we must consider systems in a holistic *** designed adequately,the hybridisation of power sources within automotive applications has been demonstrated to positively impact fuel cell efficiency,durability,and cost,while having potential benefits for the safety of *** this paper,the impact of the fuel cell to battery hybridisation degree is explored through the key design parameter of system *** fuel cell electric hybrid vehicle(FCHEV)scenarios of various hydridisation degrees,including light-duty vehicles(lDVs),Class 8 heavy goods vehicles(HGVs),and buses are modelled to enable the appropriate sizing of the proton exchange membrane(PEMFC)stack and lithium-ion battery(liB)pack and additional balance of *** operating conditions of the modelled PEMFC stack and battery pack are then varied under a range of relevant drive cycles to identify the relative performance of the *** extending the model further and incorporating a feedback loop,we are able to remove the need to include estimated vehicle masses a priori enabling improving the speed and accuracy of the model as an analysis tool for vehicle mass and performance estimation.

关键词： Proton exchange membrane(PEMFC) lithium-ion batteries fuel cell electric hybrid vehicle(FCHEV) electric propulsion powertrain modelling

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Hybrid Ni_(2)P/CoP Nanosheets as Efficient and Robust Electrocatalysts for Domestic Wastewater Splitting

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Energy & Environmental Materials 2023年第5期6卷 330-339页

作者： Yeshu Tan jianrui Feng liqun Kang longxiang liu Fangjia Zhao Siyu Zhao dan j.l.brett Paul R.Shearing Guanjie He Ivan P.Parkin Christopher Ingold laboratory Department of ChemistryUniversity College LondonLondon WC1H 0AJUK Materials and Catalysis laboratory Department of Chemical EngineeringUniversity College LondonLondon WC1E 7JEUK Electrochemical Innovation laboratory Department of Chemical EngineeringUniversity College LondonLondon WC1E 7JEUK School of Chemistry University of LincolnJoseph Banks LaboratoriesLincolnLN67DLUK

The development of low-cost,robust and efficient non-noble metal electrocatalysts is still a pursuit for the hydrogen evolution reaction(HER).Herein,a self-standing electrocatalyst,Ni_(2)P/CoP nanosheet,was fabricated directly on three-dimensional Ni foams by two facile steps,which illustrated both high activity and stability for HER in different *** from the porous structures of nanosheets with large specific surface area and the hybrid Ni_(2)P/CoP,the as-prepared electrocatalyst presented remarkable HER with overpotentials of 65.2 and 87.8 mV to reach a current density of-10 mA cm^(-2)in neutral and alkaline media,*** function theory calculations revealed a lower activation energy of water dissociation and efficient HER steps of hybrid Ni_(2)P/CoP nanosheets compared with mono *** self-standing electrocatalyst maintained excellent chemical ***,the HER process in domestic wastewater was realized with more impressive performance by using Ni_(2)P/CoP nanosheets compared with commercial Pt/*** was continuously generated for 20 h in mildly alkaline dishwashing *** work provides a feasible way to fabricate non-noble metal and self-standing hybrid bimetallic phosphides for HER in neutral and alkaline media,showing great potential for efficient hydrogen production by re-utilizing wastewater resources.

关键词： hybrid hydrogen evolution reaction Ni_(2)P/CoP nanosheet self-standing wastewater splitting

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Reversible lithium storage in sp^(2) hydrocarbon frameworks

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journal of Energy Chemistry 2022年第3期31卷 161-167,I0006页

作者： Zhangxiang Hao junrun Feng Yiyun liu liqun Kang Bolun Wang junwen Gu lin Sheng Ruoyu Xu Sushila Marlow dan j.l.brett Yunhui Huang Feng Ryan Wang Materials and Catalysis laboratory Department of Chemical EngineeringUniversity College LondonLondon WC1E 7JEUnited Kingdom School of Materials Science and Engineering Huazhong University of Science and TechnologyWuhan 430074HubeiChina Electrochemical Innovation lab Department of Chemical EngineeringUniversity College LondonLondon WC1E 7JEUnited Kingdom Department of Chemistry University College LondonLondon WC1H 0AJUnited Kingdom

Polymer materials offer controllable structure-dependent performances in separation,catalysis and drug *** molecular structures can be precisely tailored to accept li^(+)for energy storage *** the design of sp^(2)carbon-based polyphenylene(PPH)with high lithium-ion uptakes and long-term stability is ***-PPH(l-PPH)exceeds the performance of crosslink-PPH(C-PPH),due to the fact that it has an ordered lamellar structure,promoting the li^(+)intercalation/deintercalation *** l-PPH cell shows a clear charge and discharge plateau at 0.35 and 0.15 V ***^(+)/li,respectively,which is absent in the C-PPH *** li^(+)storage capacity of l-PPH is five times that of the *** reversible storage capacity is further improved to 261 m Ah g;by functionalizing the l-PPH with the–SO_(3)H *** addition,the li-intercalated structures of C-PPH and l-PPH are investigated via near-edge X-ray absorption fine structure(NEXAFS),suggesting the high reversible li^(+)–C=C bond interaction at *** strategy,based on new insight into sp^(2)functional groups,is the first step toward a molecular understanding of the structure storage-capacity relationship in sp^(2)carbon-based polymer.

关键词： lithium-ions battery Organic anode Topological structure sp^(2)hydrocarbon

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Battery state-of-charge estimation using machine learning analysis of ultrasonic signatures

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Energy and AI 2022年第4期10卷 60-72页

作者： Elias Galiounas Tom G.Tranter Rhodri E.Owen james B.Robinson Paul R.Shearing dan j.l.brett Electrochemical Innovation lab Department of Chemical EngineeringUniversity College LondonLondonWC1E 7JEUK The Faraday Institution Quad OneBecquerel AvenueHarwell CampusDidcotOX11 The Alan Turing Institute British Library96 Euston RoadLondon NW12DB

The potential of acoustic signatures to be used for State-of-Charge(SoC)estimation is demonstrated using artificial neural network regression *** approach represents a streamlined method of processing the entire acoustic waveform instead of performing manual,and often arbitrary,waveform peak *** applications where computational economy is prioritised,simple metrics of statistical significance are used to formally identify the most informative waveform *** alone can be exploited for SoC *** is further shown that signal portions representing both early and late interfacial reflections can correlate highly with the SoC and be of predictive value,challenging the more common peak selection methods which focus on the *** later echoes represent greater through-thickness coverage,and are intuitively more information-rich,their presence is not *** waveform treatment offers a more robust approach to correlating acoustic signatures to electrochemical *** is further demonstrated that transformation into the frequency domain can reduce the dimensionality of the problem significantly,while also improving the estimation *** importantly,it is shown that acoustic signatures can be used as sole model inputs to produce highly accurate SoC estimates,without any complementary voltage *** makes the method suitable for applications where redundancy and diversification of SoC estimation approaches is *** is obtained experimentally from a 210 mAh liCoO2/graphite pouch *** estimation errors as low as 0.75%are achieved on a SoC scale of 0-100%.

关键词： Battery diagnostics Ultrasonic battery monitoring Acoustic battery inspection Mechanical-electrochemical correlation Machine learning Artificial neural networks

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Sodium Superionic Conductors(NASICONs)as Cathode Materials for Sodium‑Ion Batteries

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Electrochemical Energy Reviews 2021年第4期4卷 793-823页

作者： Qingbo Zhou linlin Wang Wenyao li Kangning Zhao Minmin liu Qian Wu Yujie Yang Guanjie He Ivan P.Parkin Paul R.Shearing dan j.l.brett jiujun Zhang Xueliang Sun Institute for Sustainable Energy/College of Sciences Shanghai UniversityShanghai 200444China Electrochemical Innovation lab Department of Chemical EngineeringUniversity College LondonLondon WC1E 7JEUK laboratory of Advanced Separations(lAS) Ecole Polytechnique Federale de Lausanne(EPFL)1950 SionSwitzerland Department of Mechanical and Materials Engineering University of Western OntarioLondonON N6A 3K7Canada

Sodium-ion batteries(SIBs)have developed rapidly owing to the high natural abundance,wide distribution,and low cost of *** the various materials used in SIBs,sodium superion conductor(NASICON)-based electrode materials with remarkable structural stability and high ionic conductivity are one of the most promising candidates for sodium storage ***,the relatively low electronic conductivity of these materials makes them display poor electrochemical performance,significantly limiting their practical *** recent years,the strategies of enhancing the inherent conductivity of NASICON-based cathode materials have been extensively studied through coating the active material with a conductive carbon layer,reducing the size of the cathode material,combining the cathode material with various carbon materials,and doping elements in the bulk *** this paper,we review the recent progress in the development of NASICON-based cathode materials for SIBs in terms of their synthesis,characterization,functional mechanisms,and performance validation/*** advantages and disadvantages of such SIB cathode materials are analyzed,and the relationship between electrode structures and electrochemical performance as well as the strategies for enhancing their electrical conductivity and structural stability is *** technical challenges of NASICON-based cathode materials with respect to SIB performance are analyzed,and several future research directions are also proposed for overcoming the challenges toward practical applications.

关键词： Sodium-ion battery Cathode materials Energy storage Sodium superionic conductor(NASICON)

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Electrospinning as a route to advanced carbon fibre materials for selected low-temperature electrochemical devices:A review

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journal of Energy Chemistry 2021年第8期30卷 492-529,I0011页

作者： Yue Wen Matt D.R.Kok jorge Pavel Victoria Tafoya Ana Bjorge Sobrido Ellsworth Bell jeff T.Gostick Servann Herou Philipp Schlee Maria-Magdalena Titirici dan j.l.brett Paul R.Shearing Rhodri jervis The Electrochemical Innovation lab Dept.of Chemical EngineeringUniversity College LondonTorrington PlaceWC1E 7JE LondonUK Queen Mary University of london School of Engineering and Materials ScienceMile End RoadE14NS LondonUK Department of Chemical Engineering University of WaterlooWaterlooCanada Department of Chemical Engineering Imperial College LondonSouth Kensington CampusSW72AZ LondonUK

Electrospinning has been proven as a highly versatile fabrication method for producing nano-structured fibres with controllable morphology,of both the fibres themselves and the void structure of the ***,it is possible to use heteroatom doped polymers or to include catalytic precursors in the electrospinning solution to control the surface properties of the *** factors make it an ideal method for the production of electrodes and flow media for a variety of electrochemical devices,enabling reduction in mass transport and activation overpotentials and therefore increasing ***,the use of biomass as a polymer source has recently gained attention for the ability to embed sustainable principles in the materials of electrochemical devices,complementing their ability to allow an increase in the use of renewable electricity via their *** this review,the historical and recent developments of electrospun materials for application in redox flow batteries,fuel cells,metal air batteries and supercapacitors are thoroughly reviewed,including an overview of the electrospinning process and a guide to best ***,we provide an outlook for the emerging use of this process in the field of electrochemical energy devices with the hope that the combination of tailored microstructure,surface functionality and computer modelling will herald a new era of bespoke functional materials that can significantly improve the performance of the devices in which they are used.

关键词： Electrospinning Redox flow batteries Fuel cells Metal-air batteries Supercapacitors

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