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Controlled Synthesis of Copper Sulfide-associated Catalysts for Electrochemical Reduction of CO2 to Formic Acid and Beyond: A Review 用于将二氧化碳电化学还原为甲酸及其他物质的硫化铜相关催化剂的可控合成:综述
Energy advances Pub Date : 2024-09-03 DOI: 10.1039/d4ya00302k
Anirban Mukherjee, Maryam Abdinejad, Susanta Sinha Mahapatra, Bidhan Chandra Ruidas
{"title":"Controlled Synthesis of Copper Sulfide-associated Catalysts for Electrochemical Reduction of CO2 to Formic Acid and Beyond: A Review","authors":"Anirban Mukherjee, Maryam Abdinejad, Susanta Sinha Mahapatra, Bidhan Chandra Ruidas","doi":"10.1039/d4ya00302k","DOIUrl":"https://doi.org/10.1039/d4ya00302k","url":null,"abstract":"Converting carbon dioxide (CO2) into value-added chemicals is considered as a promising strategy to mitigate climate change. Among the various CO2 reduction techniques, electrochemical CO2 reduction (ERCO2) using renewable energy sources holds significant potential. Consequently, the design and development of electrocatalysts capable of offering both high performance and cost-effectiveness hold the potential to expedite reaction kinetics and facilitate widespread industrial adoption. In recent years, abundant copper sulfide (Cu/S)-associated nanomaterials among various metal-chalcogenides have been of extensive research interest due to their semiconductor and low toxicity properties, enabling them to be used in widespread applications of the ERCO2 field. This review highlights the progress of engineered Cu/S-associated nanomaterials for ERCO2 reactions and elaborates on the correlations of engineering strategies, catalytic activity, and reaction pathways. The paper also summarises the controllable synthesis methods for fabricating various state-of-the-art Cu/S-associated structures and outlines their possible implementation for CO2 reduction as an electrocatalyst. Finally, challenges and prospects are presented for the future development and practical application of Cu/S-associated catalysts for ECO2R to value-added chemicals.","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142207375","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Electricity generation using a microbial 3D bio-anode embedded bio-photovoltaic cell in a microfluidic chamber 利用微流控室中的微生物三维生物阳极嵌入式生物光伏电池发电
Energy advances Pub Date : 2024-09-03 DOI: 10.1039/d4ya00278d
Zülal Muganlı, İsmail Bütün, Ghazaleh Gharib, Ali Koşar
{"title":"Electricity generation using a microbial 3D bio-anode embedded bio-photovoltaic cell in a microfluidic chamber","authors":"Zülal Muganlı, İsmail Bütün, Ghazaleh Gharib, Ali Koşar","doi":"10.1039/d4ya00278d","DOIUrl":"https://doi.org/10.1039/d4ya00278d","url":null,"abstract":"New-generation sustainable energy systems serve as major tools to mitigate the greenhouse gas emissions and effects of climate change. Biophotovoltaics (BPVs) presents an eco-friendly approach by employing solar energy to ensure self-sustainable bioelectricity. In contrast to other microbial fuel cells (MFCs), carbon feedstock is not essential for generating electricity with BPVs. However, the low power outputs (μW cm<small><sup>−2</sup></small>) obtained from the current systems limit their practical applications. In this study, a new generation polydimethylsiloxane (PDMS) based BPV cell unit was developed with a 3D hydrogel scaffold-based bio-anode to enable microbial biofilm formation for substantial electron capture and extracellular electron transfer. Moreover, the fabricated device was supported using an air-cathode electrode to elevate the gas exchange, thereby enabling optimum photosynthesis. <em>Synechocystis</em> sp. PCC 6803 seeded the 3D bio-anode embedded BPV cell, whose electrical characteristics were analyzed under the illumination of white light as day/night cycles with continuous feeding by the microchannel. For the first five days, the results indicated that the maximum power densities were 0.0534 W m<small><sup>−2</sup></small> for dark hours and 0.03911 W m<small><sup>−2</sup></small> for light hours without causing any effect on the cellular morphology of the cyanobacteria. As a result, the developed hydrogel scaffold-based bio-anode embedded BPV cell led to higher power densities <em>via</em> enabling a simple, self-sustainable, biocompatible, and eco-friendly energy harvesting platform with a possible capability in the applications of power lab-on-a-chip (LOC), point-of-care (POC), and small-scale portable electronic devices.","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142207372","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Construction of organic inorganic hybrid composite derived from C3N5 incorporated with CeO2 for the enhanced photocatalytic hydrogen evolution 构建由 C3N5 与 CeO2 结合而成的有机无机杂化复合材料,用于增强光催化氢气进化
Energy advances Pub Date : 2024-09-03 DOI: 10.1039/d4ya00476k
Ashil Augustin, Manova Santhosh Yesupatham, M. D. Dhileepan, Sanguk Son, Ezhakudiyan Ravindran, Neppolian Bernaurdshaw, Hyoung-il Kim, Karthikeyan Sekar
{"title":"Construction of organic inorganic hybrid composite derived from C3N5 incorporated with CeO2 for the enhanced photocatalytic hydrogen evolution","authors":"Ashil Augustin, Manova Santhosh Yesupatham, M. D. Dhileepan, Sanguk Son, Ezhakudiyan Ravindran, Neppolian Bernaurdshaw, Hyoung-il Kim, Karthikeyan Sekar","doi":"10.1039/d4ya00476k","DOIUrl":"https://doi.org/10.1039/d4ya00476k","url":null,"abstract":"The concern regarding energy scarcity and environmental issues is effectively addressed by the photocatalytic hydrogen production. The effective combination among semiconductor materials is capable of preventing the exciton recombination, making it a method that is highly effective for enhancing photocatalytic activity. In this report, conjugated polymer encapsulated with metal oxide photocatalyst is synthesised using a simple exsitu synthesis method. The encapsulation of polymer with CeO2 nanoparticles results in exceptional performance in H2 production, as the samples exhibit improved visible light absorption and a significant increase in charge transfer efficiency. This is accredited to the high charge transfer and reduced recombination in the composite. The efficient transfer of photogenerated holes has resulted in a substantial decline in the recombination rate of excitons, and the rate of photocatalytic H2 production has been substantially enhanced. The results indicated that the hydrogen evolution of 10 wt.% CeO2/C3N5 composites was 1256 μmol/g/h, whereas C3N5 was 125 μmol/g/h. The electrochemical analysis showed that the optimised composites have low electron hole recombination rate and improved visible light absorption, thereby exhibiting excellent photocatalytic activity. It is noteworthy that the proposed research is the first study to report on the hydrogen evolution via photocatalysis using CeO2/C3N5 composites. Consequently, this research offers a new perspective on the design of organic inorganic heterostructures and will provide a novel pathway to their catalytic capabilities.","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142207345","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Novel carbon-free innovation in centralised ammonia cracking for a sustainable hydrogen economy: the hybrid air-volt ammonia cracker (HAVAC) process 用于可持续氢经济的集中式氨裂解无碳创新技术:混合气体-电压氨裂解工艺(HAVAC)
Energy advances Pub Date : 2024-09-03 DOI: 10.1039/d4ya00483c
Chidozie Eluwah, Paul S. Fennell
{"title":"Novel carbon-free innovation in centralised ammonia cracking for a sustainable hydrogen economy: the hybrid air-volt ammonia cracker (HAVAC) process","authors":"Chidozie Eluwah, Paul S. Fennell","doi":"10.1039/d4ya00483c","DOIUrl":"https://doi.org/10.1039/d4ya00483c","url":null,"abstract":"The hybrid air-volt ammonia cracker (HAVAC) represents a novel approach to centralised ammonia cracking for hydrogen production, enhancing both efficiency and scalability. This novel process integrates renewable electricity and autothermal operation to crack blue or green ammonia, achieving a high thermal efficiency of 94% to 95%. HAVAC demonstrates impressive ammonia conversion rates up to 99.4% and hydrogen yields between 84% and 99.5%, with hydrogen purity of 99.99% meeting ISO 14687:2019 standards. Key innovations include the process's flexibility to operate in three modes: 100% renewable electricity, 100% air autothermal, or a hybrid approach. This versatility optimizes energy use and adapts to varying conditions. The gas heated cracker (GHC) within HAVAC efficiently reduces energy demands by utilizing waste heat. Modelled using the Aspen Plus Simulator and validated against experimental data, HAVAC's economic analysis indicates a levelized cost of hydrogen (LCOH) between $3.80 per kg-H<small><sub>2</sub></small> and $6.00 per kg-H<small><sub>2</sub></small>. The process's environmental benefits include reduced greenhouse gas emissions and effective NOx waste management. Future research will focus on scaling up, reducing ammonia feed cost, optimizing catalysts, and enhancing waste management. HAVAC offers substantial promise for advancing hydrogen production and supporting a sustainable, carbon-free hydrogen economy. The technical and economic data generated by this analysis will assist decision-makers and researchers in advancing the pursuit of a carbon-free hydrogen economy.","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142207343","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Efficiency in Photocatalytic Production of Hydrogen: Energetic and Sustainability implications 光催化制氢的效率:能源和可持续性影响
Energy advances Pub Date : 2024-09-02 DOI: 10.1039/d4ya00361f
Rocío Sayago-Carro, Luis J Jinénez-Chavarriga, Esperanza Fernández-García, Anna Kubacka, Marcos Fernández-García
{"title":"Efficiency in Photocatalytic Production of Hydrogen: Energetic and Sustainability implications","authors":"Rocío Sayago-Carro, Luis J Jinénez-Chavarriga, Esperanza Fernández-García, Anna Kubacka, Marcos Fernández-García","doi":"10.1039/d4ya00361f","DOIUrl":"https://doi.org/10.1039/d4ya00361f","url":null,"abstract":"Hydrogen generation through a photocatalytic process appears a promising technology to produce this energy vector through a novel, efficient, green, and sustainable process. The fruitful use of sunlight as excitation source and renewable bio-derived reactants as well as the development of highly efficient catalysts are required to achieve this goal. In this perspective article, we focus on describing how to braid energy and sustainability sides of the hydrogen photo-generation into a single parameter, allowing quantitative measurement and trustful comparison of different catalytic systems. Starting from the energy-related efficiency parameters defined by the IUPAC, we present novel approaches leading to parameters enclosing energy and sustainability information. The study is completed with the analysis of other, non-IUPAC, parameters of broad use such as the Solar-to-Hydrogen observable. To set of results available in the literature for the water splitting reaction and the use of bio-derived sacrificial molecules is reviewed to assess the potential of such reactions in the energy-efficient and sustainable production of hydrogen.","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142207374","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Correction: Acid–base concentration swing for direct air capture of carbon dioxide 更正:直接空气捕集二氧化碳的酸碱浓度摆动
IF 3.2
Energy advances Pub Date : 2024-08-30 DOI: 10.1039/D4YA90035A
Anatoly Rinberg and Michael J. Aziz
{"title":"Correction: Acid–base concentration swing for direct air capture of carbon dioxide","authors":"Anatoly Rinberg and Michael J. Aziz","doi":"10.1039/D4YA90035A","DOIUrl":"https://doi.org/10.1039/D4YA90035A","url":null,"abstract":"<p >Correction for ‘Acid–base concentration swing for direct air capture of carbon dioxide’ by Anatoly Rinberg and Michael J. Aziz, <em>Energy Adv.</em>, 2024, https://doi.org/10.1039/d4ya00251b.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":null,"pages":null},"PeriodicalIF":3.2,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ya/d4ya90035a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142174073","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Anion exchange membrane water electrolysis over superparamagnetic ferrites 超顺磁性铁氧体上的阴离子交换膜电解水
Energy advances Pub Date : 2024-08-30 DOI: 10.1039/d4ya00170b
Tiago Fernandes, Ramsundar Rani Mohan, Laura Donk, Wei Chen, Chiara Biz, Mauro Fianchini, Saeed Kamali, Siavash Mohammad Alizadeh, Anna Kitayev, Aviv Ashdot, Miles Page, Laura M. Salonen, Sebastian Kopp, Ervin Tal Gutelmacher, José Gracia, Marta Costa Figueiredo, Yury V. Kolen’ko
{"title":"Anion exchange membrane water electrolysis over superparamagnetic ferrites","authors":"Tiago Fernandes, Ramsundar Rani Mohan, Laura Donk, Wei Chen, Chiara Biz, Mauro Fianchini, Saeed Kamali, Siavash Mohammad Alizadeh, Anna Kitayev, Aviv Ashdot, Miles Page, Laura M. Salonen, Sebastian Kopp, Ervin Tal Gutelmacher, José Gracia, Marta Costa Figueiredo, Yury V. Kolen’ko","doi":"10.1039/d4ya00170b","DOIUrl":"https://doi.org/10.1039/d4ya00170b","url":null,"abstract":"The oxygen evolution reaction (OER) is usually the bottleneck in water electrolysis due to its sluggish kinetics, resulting in increased costs in the production of green hydrogen. Therefore, there is a need for more efficient, stable, and ideally, critical-raw-material-free catalysts. To this end, we have synthesized nanosized spinel ferrites CoFe<small><sub>2</sub></small>O<small><sub>4</sub></small>, NiFe<small><sub>2</sub></small>O<small><sub>4</sub></small>, and ZnFe<small><sub>2</sub></small>O<small><sub>4</sub></small>, and a high-entropy spinel ferrite Zn<small><sub>0.2</sub></small>Mn<small><sub>0.2</sub></small>Ni<small><sub>0.2</sub></small>Co<small><sub>0.2</sub></small>Fe<small><sub>2.2</sub></small>O<small><sub>4</sub></small> through a simple coprecipitation reaction in an automated reactor on a gram scale. The powder X-ray diffraction and transmission electron microscopy studies revealed crystallite sizes of 20–35 nm. Insight into the oxidation states and cation distribution in the mixed spinel systems was gained through X-ray photoelectron and Mössbauer spectroscopy studies. The activity of all spinel ferrites was tested for the OER through half-cell laboratory measurements and full-cell anion exchange membrane electrolysis (AEMEL), where Zn<small><sub>0.2</sub></small>Mn<small><sub>0.2</sub></small>Ni<small><sub>0.2</sub></small>Co<small><sub>0.2</sub></small>Fe<small><sub>2.2</sub></small>O<small><sub>4</sub></small> showed the lowest overpotential of 432 mV at a current density of 10 mA cm<small><sup>−2</sup></small>. All the synthesized ferrites demonstrated good stability up to 20 h, with NiFe<small><sub>2</sub></small>O<small><sub>4</sub></small> being the most active in high current density experiments up to 2 A cm<small><sup>−2</sup></small>. In addition, studies on the magnetic properties at room temperature revealed a largely superparamagnetic response of the prepared materials, indicating that quantum spin-exchange interactions facilitate oxygen electrochemistry. Computational calculations shed light on the superior catalytic activities of NiFe<small><sub>2</sub></small>O<small><sub>4</sub></small> and Zn<small><sub>0.2</sub></small>Mn<small><sub>0.2</sub></small>Ni<small><sub>0.2</sub></small>Co<small><sub>0.2</sub></small>Fe<small><sub>2.2</sub></small>O<small><sub>4</sub></small>, the two strongly correlated oxides that exhibit the highest magnetization and the smallest band gaps, corroborating the recent principles determining the activity of magnetic oxides in electron transfer reactions.","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142207380","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Direct formate anion exchange membrane fuel cells with a PdAu bimetallic nanoparticle anode electrocatalyst obtained by metal vapor synthesis 采用通过金属蒸气合成获得的 PdAu 双金属纳米粒子阳极电催化剂的直接甲酸阴离子交换膜燃料电池
Energy advances Pub Date : 2024-08-29 DOI: 10.1039/d4ya00324a
Carolina Castello, Tailor Peruzzolo, Marco Bellini, Maria V. Pagliaro, Francesco Bartoli, Enrico Berretti, Lorenzo Poggini, Emanuela Pitzalis, Claudio Evangelisti, Hamish A. Miller
{"title":"Direct formate anion exchange membrane fuel cells with a PdAu bimetallic nanoparticle anode electrocatalyst obtained by metal vapor synthesis","authors":"Carolina Castello, Tailor Peruzzolo, Marco Bellini, Maria V. Pagliaro, Francesco Bartoli, Enrico Berretti, Lorenzo Poggini, Emanuela Pitzalis, Claudio Evangelisti, Hamish A. Miller","doi":"10.1039/d4ya00324a","DOIUrl":"https://doi.org/10.1039/d4ya00324a","url":null,"abstract":"Fuels can be produced from the electrochemical reduction of industrial waste CO<small><sub>2</sub></small> (e-fuels) using renewable energy and hence are an attractive option for the storage of renewable energy in a chemical form. The energy stored in the e-Fuel may be recovered on-demand using a direct fuel cell thus completing a carbon neutral cycle. Anion exchange membrane fuel cells (AEMFCs) are versatile devices that can be fed by both a gaseous fuel such as H<small><sub>2</sub></small> and with liquid fuels (<em>e.g.</em> alcohols, formate, hydrazine, NaBH<small><sub>4</sub></small>). Formate is a molecule that can be easily obtained by the electrochemical reduction of CO<small><sub>2</sub></small> with high selectivity. Efficient re-transformation of the energy stored in the chemical bonds into electrical energy requires the development of efficient and stable electrocatalysts. Palladium alloy catalysts are highly active under alkaline conditions when Pd is mixed with more oxophilic transition metals. Here we report that enhanced activity and stability can be obtained with Au–Pd alloy nanoparticles when compared to a Pd catalyst. Both catalysts are prepared by a metal vapour synthesis method. We show that the key to enhanced performance is the partial segregation of Au to the NP surface that increases oxophilicity and favours the adsorption and transfer of OH<small><sup>−</sup></small> species to the active Pd sites. This enhanced activity translates to high power densities and performance stability when employed in AEMFCs fed with aqueous potassium formate fuel (Peak power density of 0.14 W cm<small><sup>−2</sup></small>, energy efficiency of 33%, faradaic efficiency of 80%).","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142207373","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Quantitative local state of charge mapping by operando electrochemical fluorescence microscopy in porous electrodes 通过多孔电极中的操作电化学荧光显微镜绘制定量局部电荷状态图
Energy advances Pub Date : 2024-08-28 DOI: 10.1039/d4ya00362d
Anton M. Graf, Thomas Cochard, Kiana Amini, Michael S. Emanuel, Shmuel M. Rubinstein, Michael J. Aziz
{"title":"Quantitative local state of charge mapping by operando electrochemical fluorescence microscopy in porous electrodes","authors":"Anton M. Graf, Thomas Cochard, Kiana Amini, Michael S. Emanuel, Shmuel M. Rubinstein, Michael J. Aziz","doi":"10.1039/d4ya00362d","DOIUrl":"https://doi.org/10.1039/d4ya00362d","url":null,"abstract":"We introduce <em>operando</em> quantitative electrochemical fluorescence state of charge mapping (QEFSM), a non-invasive technique to study operating electrochemical systems along with a new design of optically transparent microfluidic redox flow cells compatible with the most demanding optical requirements. QEFSM allows quantitative mappings of the concentration of a particular oxidation state of a redox-active species within a porous electrode during its operation. In this study, we used confocal microscopy to map the fluorescence signal of the reduced form of 2,7-anthraquinone disulfonate (AQDS) in a set of multistep-chronoamperometry experiments. Calibrating these images and incorporating an analytical model of quinhydrone heterodimer formation with no free parameters, and accounting for the emission of each species involved, we determined the local molecular concentration and the state of charge (SOC) fields within a commercial porous electrode during operation. With this method, electrochemical conversion and species advection, reaction and diffusion can be monitored at heretofore unprecedented transverse and axial resolution (1 μm and 25 μm, respectively) at frame rates of 0.5 Hz, opening new routes to understanding local electrochemical processes in porous electrodes. We observed pore-scale SOC inhomogeneities appearing when the fraction of electroactive species converted in a single pass through the electrode becomes large.","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142207378","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Ion-conductive vs. non-ion-conductive ceramic fillers in silane-linked polyethylene oxide-based composite polymer electrolytes with high room-temperature ionic conductivity 具有高室温离子导电性的硅烷连接聚乙烯氧化物基复合聚合物电解质中的离子导电与非离子导电陶瓷填料
Energy advances Pub Date : 2024-08-28 DOI: 10.1039/d4ya00231h
Eun Ju Jeon, Sharif Haidar, Laura Helmers, Arno Kwade, Georg Garnweitner
{"title":"Ion-conductive vs. non-ion-conductive ceramic fillers in silane-linked polyethylene oxide-based composite polymer electrolytes with high room-temperature ionic conductivity","authors":"Eun Ju Jeon, Sharif Haidar, Laura Helmers, Arno Kwade, Georg Garnweitner","doi":"10.1039/d4ya00231h","DOIUrl":"https://doi.org/10.1039/d4ya00231h","url":null,"abstract":"Polyethylene oxide (PEO)-based polymer electrolytes, despite their cost-effectiveness and ease of processing, suffer from low ionic conductivity at lower temperatures due to the semi-crystalline nature of PEO. Incorporating ceramic filler particles into the polymer matrix offers a potential solution by disrupting its rigid crystalline structure, thereby improving the flexibility of the polymer chains. However, the Li ion conduction pathway within these composite polymer electrolytes (CPEs) remains predominantly within the polymer matrix if the filler particles are only physically mixed. The surface modification of filler particles can improve the interfacial compatibility and ionic conductivity. In this work, two types of filler particles, passive ZrO<small><sub>2</sub></small> and active Li<small><sub>7</sub></small>La<small><sub>3</sub></small>Zr<small><sub>2</sub></small>O<small><sub>12</sub></small> (LLZO), are compared and incorporated into PEO–polyethylene glycol (PEG)–lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) CPEs. The surface of the filler particles is functionalized with a silane ligand ((3-glycidyloxypropyl)trimethoxysilane (GPTMS)) prior to their integration into the PEO matrix. This modifies the interfacial properties between the polymer and the filler particles, hence influencing the ionic conductivity. The functionalized ZrO<small><sub>2</sub></small> fillers enhance the ionic conductivity of the CPEs by reducing the crystallinity of PEO. The PEO–PEG–LiTFSI CPE with 15 vol% of GPTMS–ZrO<small><sub>2</sub></small> achieved an ionic conductivity of 6.66 × 10<small><sup>−4</sup></small> S cm<small><sup>−1</sup></small> at 20 °C, which is significantly higher than that of the standard PEO–LiTFSI (9.26 × 10<small><sup>−6</sup></small> S cm<small><sup>−1</sup></small>). Additionally, coupling GPTMS to PEO chains without the introduction of filler particles also improved the ionic conductivity, while the incorporation of functionalized LLZO fillers does not, which is attributed to a LiCO<small><sub>3</sub></small> passivation layer. The results suggest a viable strategy to overcome the inherent limitations of PEO electrolyte, thus offering valuable insights into the design and optimization of CPEs for practical applications.","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142207377","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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