Pub Date : 2025-02-01DOI: 10.1016/j.coelec.2024.101628
Anousha Sohail, Chularat Wattanakit
Rising concerns over fossil fuel reliance have driven the development of biomass-derived chemical production. Transforming hydroxymethylfurfural (HMF) and furfural, key platform compounds, into sustainable chemicals enhances the biomass value chain. Electrosynthesis emerges as a green and efficient approach to upgrading furan derivatives into biofuels, biopolymers, and industrial chemicals. This minireview discusses advancements in electrocatalytic upgrading of furan derivatives, particularly featuring biorefinery with hydrogen production for cost-efficient and sustainable processes. Importantly, this minireview also highlights the current advancement in electrocatalyst design and addresses the challenges of improving electrocatalytic efficiency in terms of enhanced product selectivity, Faradaic efficiency (FE), and overall process sustainability.
{"title":"Electrocatalytic upgrading of furan derivatives","authors":"Anousha Sohail, Chularat Wattanakit","doi":"10.1016/j.coelec.2024.101628","DOIUrl":"10.1016/j.coelec.2024.101628","url":null,"abstract":"<div><div>Rising concerns over fossil fuel reliance have driven the development of biomass-derived chemical production. Transforming hydroxymethylfurfural (HMF) and furfural, key platform compounds, into sustainable chemicals enhances the biomass value chain. Electrosynthesis emerges as a green and efficient approach to upgrading furan derivatives into biofuels, biopolymers, and industrial chemicals. This minireview discusses advancements in electrocatalytic upgrading of furan derivatives, particularly featuring biorefinery with hydrogen production for cost-efficient and sustainable processes. Importantly, this minireview also highlights the current advancement in electrocatalyst design and addresses the challenges of improving electrocatalytic efficiency in terms of enhanced product selectivity, Faradaic efficiency (FE), and overall process sustainability.</div></div>","PeriodicalId":11028,"journal":{"name":"Current Opinion in Electrochemistry","volume":"49 ","pages":"Article 101628"},"PeriodicalIF":7.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143164165","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.coelec.2024.101611
Dipam Manish Patel, Anjana Tripathi, Vivianne Karina Ocampo-Restrepo, Georg Kastlunger
The reversible and computational hydrogen electrodes have proven invaluable as reference electrodes in aqueous electrocatalysis, allowing an evaluation of the combined chemical potential of the proton–electron pair in experiments and computations. By construction, they cancel the pH dependence in most capacitive processes. However, for electrocatalysis, which is dominated by faradaic processes, this characteristic is rarely observed.
In this short review, we discuss the origins of deviations from the Nernstian behavior in capacitive and faradaic processes, their manifestation in experimental observables, and attempts to incorporate them in simulations. On this basis, we discuss how deviations from Nernstian behavior can be exploited in mechanistic analysis and highlight the use of electrostatic descriptors in computational screening to account for non-Nernstian effects explicitly.
{"title":"Electrocatalysis beyond the reversible hydrogen electrode","authors":"Dipam Manish Patel, Anjana Tripathi, Vivianne Karina Ocampo-Restrepo, Georg Kastlunger","doi":"10.1016/j.coelec.2024.101611","DOIUrl":"10.1016/j.coelec.2024.101611","url":null,"abstract":"<div><div>The reversible and computational hydrogen electrodes have proven invaluable as reference electrodes in aqueous electrocatalysis, allowing an evaluation of the combined chemical potential of the proton–electron pair in experiments and computations. By construction, they cancel the pH dependence in most capacitive processes. However, for electrocatalysis, which is dominated by faradaic processes, this characteristic is rarely observed.</div><div>In this short review, we discuss the origins of deviations from the Nernstian behavior in capacitive and faradaic processes, their manifestation in experimental observables, and attempts to incorporate them in simulations. On this basis, we discuss how deviations from Nernstian behavior can be exploited in mechanistic analysis and highlight the use of electrostatic descriptors in computational screening to account for non-Nernstian effects explicitly.</div></div>","PeriodicalId":11028,"journal":{"name":"Current Opinion in Electrochemistry","volume":"49 ","pages":"Article 101611"},"PeriodicalIF":7.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143102844","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.coelec.2024.101615
Kayvan Moradi, Marko M. Melander
Semiconductor electrodes (SCEs) play a decisive role in clean energy conversion technologies but understanding their complex electrochemistry remains an outstanding challenge. Herein, we review electronic structure methods for describing the applied electrode potential in simulations of semiconductor–electrolyte interfaces. We emphasize that inclusion of the electrode potential is significantly more challenging for SCEs than for metallic electrodes because SCEs require accurate models of semiconductor capacitance, including the space-charge region and surface effects, as well as the electrolyte double-layer capacitance. We discuss how these physicochemical complications challenge the development of atomistic models of SCE and how they impact the applicability of the computational hydrogen electrode, capacitance correction, grand canonical DFT, and Green function methods to model SCEs. We highlight the need for continued methodological development and conclude that integrating advanced atomistic models of SCEs with grand canonical, constant inner potential DFT or Green function methods holds promise for accurate SCE simulations.
{"title":"Electronic structure methods for simulating the applied potential in semiconductor electrochemistry","authors":"Kayvan Moradi, Marko M. Melander","doi":"10.1016/j.coelec.2024.101615","DOIUrl":"10.1016/j.coelec.2024.101615","url":null,"abstract":"<div><div>Semiconductor electrodes (SCEs) play a decisive role in clean energy conversion technologies but understanding their complex electrochemistry remains an outstanding challenge. Herein, we review electronic structure methods for describing the applied electrode potential in simulations of semiconductor–electrolyte interfaces. We emphasize that inclusion of the electrode potential is significantly more challenging for SCEs than for metallic electrodes because SCEs require accurate models of semiconductor capacitance, including the space-charge region and surface effects, as well as the electrolyte double-layer capacitance. We discuss how these physicochemical complications challenge the development of atomistic models of SCE and how they impact the applicability of the computational hydrogen electrode, capacitance correction, grand canonical DFT, and Green function methods to model SCEs. We highlight the need for continued methodological development and conclude that integrating advanced atomistic models of SCEs with grand canonical, constant inner potential DFT or Green function methods holds promise for accurate SCE simulations.</div></div>","PeriodicalId":11028,"journal":{"name":"Current Opinion in Electrochemistry","volume":"49 ","pages":"Article 101615"},"PeriodicalIF":7.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143102845","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.coelec.2024.101613
Eric Labbé, Olivier Buriez
The introduction of light absorption steps in organic and organometallic synthetic processes has enlarged the scope of accessible intermediates, featuring photoexcited species with both strong reducing and oxidizing properties. Nowadays, two approaches use the absorption of visible light to carry out new organic reactions, namely photoredox catalysis and electrophotocatalysis. The intent of this review is to show how molecular electrochemistry can be a powerful analytical technique for obtaining thermodynamic and kinetic information in these new light-integrated reactions, and also constitute a complementary approach to photochemical investigations. The development of reactions involving a photoactivation step should strengthen the links between the photochemical and electrochemical communities.
{"title":"Interplay between molecular electrochemistry and light in mechanistic investigations","authors":"Eric Labbé, Olivier Buriez","doi":"10.1016/j.coelec.2024.101613","DOIUrl":"10.1016/j.coelec.2024.101613","url":null,"abstract":"<div><div>The introduction of light absorption steps in organic and organometallic synthetic processes has enlarged the scope of accessible intermediates, featuring photoexcited species with both strong reducing and oxidizing properties. Nowadays, two approaches use the absorption of visible light to carry out new organic reactions, namely photoredox catalysis and electrophotocatalysis. The intent of this review is to show how molecular electrochemistry can be a powerful analytical technique for obtaining thermodynamic and kinetic information in these new light-integrated reactions, and also constitute a complementary approach to photochemical investigations. The development of reactions involving a photoactivation step should strengthen the links between the photochemical and electrochemical communities.</div></div>","PeriodicalId":11028,"journal":{"name":"Current Opinion in Electrochemistry","volume":"49 ","pages":"Article 101613"},"PeriodicalIF":7.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143102850","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.coelec.2024.101625
Yaovi Holade , Teko W. Napporn , Kouakou Boniface Kokoh
In the current context of sustainability, the selective electrocatalytic transformation of biomass-derived organic substances into value-added products should offer vast design possibilities for power generation or the electrosynthesis of fuels and commodity chemicals. In this contribution, we have examined a number of concepts concerning the electrocatalysis of organic molecules for which noble metals cannot be excluded from the electrocatalyst composition without compromising the significant energy savings promised in electrolyzers (up to 50 % for H2 co-production compared with conventional water electrolysis). The widespread practice of using the ratio of forward peak current to backward peak current as a measure of activity, anti-poison capacity or removal of adsorbed poisons or intermediates is unsuitable based on voltammetry and spectroelectrochemical analysis.
{"title":"Electrocatalysis of organics for electrolysis and/or fuel cells: Some thoughts on using the ratio of forward to backward peak current as a measure of electrocatalyst efficiency and/or poisoning","authors":"Yaovi Holade , Teko W. Napporn , Kouakou Boniface Kokoh","doi":"10.1016/j.coelec.2024.101625","DOIUrl":"10.1016/j.coelec.2024.101625","url":null,"abstract":"<div><div>In the current context of sustainability, the selective electrocatalytic transformation of biomass-derived organic substances into value-added products should offer vast design possibilities for power generation or the electrosynthesis of fuels and commodity chemicals. In this contribution, we have examined a number of concepts concerning the electrocatalysis of organic molecules for which noble metals cannot be excluded from the electrocatalyst composition without compromising the significant energy savings promised in electrolyzers (up to 50 % for H<sub>2</sub> co-production compared with conventional water electrolysis). The widespread practice of using the ratio of forward peak current to backward peak current as a measure of activity, anti-poison capacity or removal of adsorbed poisons or intermediates is unsuitable based on voltammetry and spectroelectrochemical analysis.</div></div>","PeriodicalId":11028,"journal":{"name":"Current Opinion in Electrochemistry","volume":"49 ","pages":"Article 101625"},"PeriodicalIF":7.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143102999","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Biodiesel, developed as an alternative to natural fossils, is produced by a transesterification reaction. The main co-product of this reaction is represented by glycerol, whose production in 2020 exceeded 6 times the current demand. A consequence of the spreading of biodiesel market was a drop of glycerol price. This versatile biomass-derived compound can be used as an important raw material for the manufacture of valuable chemicals including dihydroxyacetone (DHA), which is the most high-valued glycerol-derived product. Despite all the research devoted to achieve selective oxidation of the secondary alcohol group, this issue remains a scientific challenge. Among several routes for glycerol valorization, electrochemistry is an attractive process as discussed in this review. After a short introduction, which describes non-electrochemical methods, electrochemical oxidations on precious (based on Pt, Pd, Au and Ag) and non-precious metal electrocatalysts is discussed, with a specific focus on selectivity towards DHA.
{"title":"Tackling electrocatalytic oxidation of glycerol to dihydroxyacetone: A comprehensive review","authors":"Fiammetta Vitulano , Fulvio Uggeri , Luciano Lattuada , Alessandro Minguzzi , Alberto Vertova","doi":"10.1016/j.coelec.2025.101665","DOIUrl":"10.1016/j.coelec.2025.101665","url":null,"abstract":"<div><div>Biodiesel, developed as an alternative to natural fossils, is produced by a transesterification reaction. The main co-product of this reaction is represented by glycerol, whose production in 2020 exceeded 6 times the current demand. A consequence of the spreading of biodiesel market was a drop of glycerol price. This versatile biomass-derived compound can be used as an important raw material for the manufacture of valuable chemicals including dihydroxyacetone (DHA), which is the most high-valued glycerol-derived product. Despite all the research devoted to achieve selective oxidation of the secondary alcohol group, this issue remains a scientific challenge. Among several routes for glycerol valorization, electrochemistry is an attractive process as discussed in this review. After a short introduction, which describes non-electrochemical methods, electrochemical oxidations on precious (based on Pt, Pd, Au and Ag) and non-precious metal electrocatalysts is discussed, with a specific focus on selectivity towards DHA.</div></div>","PeriodicalId":11028,"journal":{"name":"Current Opinion in Electrochemistry","volume":"51 ","pages":"Article 101665"},"PeriodicalIF":7.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143453376","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.coelec.2024.101630
R. Daniel Little, Kevin D. Moeller, R. Francke
{"title":"Organic and molecular electrochemistry (2024)–Fresh impetus for organic synthesis","authors":"R. Daniel Little, Kevin D. Moeller, R. Francke","doi":"10.1016/j.coelec.2024.101630","DOIUrl":"10.1016/j.coelec.2024.101630","url":null,"abstract":"","PeriodicalId":11028,"journal":{"name":"Current Opinion in Electrochemistry","volume":"49 ","pages":"Article 101630"},"PeriodicalIF":7.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143098631","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.coelec.2024.101623
Yuqi Ma , Danlei Li
This mini review explores the effect of nanoparticle (NP) size and morphology on electrocatalytic activity, with a focus on the advancements in single-entity electrochemistry (SEE) techniques such as scanning electrochemical microscopy, scanning electrochemical cell microscopy, and single nanoparticle collision methods. These techniques provide critical insights into NP behavior, enabling the precise characterization of catalytic activity at a single-NP scale. Moreover, recent developments in coupling SEE with other techniques are also briefly discussed with a focus on enhanced mass transport and electrical contact in single-NP electrocatalysis.
{"title":"Recent advances in characterization of electrocatalytic nanoparticles at single-particle level","authors":"Yuqi Ma , Danlei Li","doi":"10.1016/j.coelec.2024.101623","DOIUrl":"10.1016/j.coelec.2024.101623","url":null,"abstract":"<div><div>This mini review explores the effect of nanoparticle (NP) size and morphology on electrocatalytic activity, with a focus on the advancements in single-entity electrochemistry (SEE) techniques such as scanning electrochemical microscopy, scanning electrochemical cell microscopy, and single nanoparticle collision methods. These techniques provide critical insights into NP behavior, enabling the precise characterization of catalytic activity at a single-NP scale. Moreover, recent developments in coupling SEE with other techniques are also briefly discussed with a focus on enhanced mass transport and electrical contact in single-NP electrocatalysis.</div></div>","PeriodicalId":11028,"journal":{"name":"Current Opinion in Electrochemistry","volume":"49 ","pages":"Article 101623"},"PeriodicalIF":7.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143098633","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.coelec.2024.101608
Wenjing Nan , Jiayang Lin , Linqi Xu , Lianhuan Han , Dongping Zhan
Single-layer graphene (SLG) is renowned for its unique electronic structure and zero band gap, which presents both opportunities and challenges in electrochemical systems, particularly due to its inherently inert heterogeneous electron transfer (HET) properties. Precisely tuning the physicochemical properties of SLG is crucial for optimizing its performance in electrochemical devices. For atomically thin SLG, subtle modifications to its electronic structure can enhance its heterogeneous charge transfer and surface reactivity effectively. Here we present a concise review on recent advances in modulating the interfacial electrochemical behavior of SLG and few-layer graphene, with a focus on defect engineering, layer number regulation, and interfacial engineering. We emphasize the impact of these strategies on modulating graphene's electronic structure, particularly concerning HET and electrochemical performance, and offer perspectives on future developments in this field.
{"title":"Modulating the interfacial electrochemical behavior of single layer graphene","authors":"Wenjing Nan , Jiayang Lin , Linqi Xu , Lianhuan Han , Dongping Zhan","doi":"10.1016/j.coelec.2024.101608","DOIUrl":"10.1016/j.coelec.2024.101608","url":null,"abstract":"<div><div>Single-layer graphene (SLG) is renowned for its unique electronic structure and zero band gap, which presents both opportunities and challenges in electrochemical systems, particularly due to its inherently inert heterogeneous electron transfer (HET) properties. Precisely tuning the physicochemical properties of SLG is crucial for optimizing its performance in electrochemical devices. For atomically thin SLG, subtle modifications to its electronic structure can enhance its heterogeneous charge transfer and surface reactivity effectively. Here we present a concise review on recent advances in modulating the interfacial electrochemical behavior of SLG and few-layer graphene, with a focus on defect engineering, layer number regulation, and interfacial engineering. We emphasize the impact of these strategies on modulating graphene's electronic structure, particularly concerning HET and electrochemical performance, and offer perspectives on future developments in this field.</div></div>","PeriodicalId":11028,"journal":{"name":"Current Opinion in Electrochemistry","volume":"49 ","pages":"Article 101608"},"PeriodicalIF":7.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143102829","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-01DOI: 10.1016/j.coelec.2024.101624
Tereza Bautkinova, Martin Prokop, Tomas Bystron, Karel Bouzek
This review examines advancements in the design of the anode porous transport layer (PTL) and catalyst layer (CL) interface in proton exchange membrane water electrolysis (PEMWE). The quality of PTL-CL interface (contact area and contact resistance per area) is critical to electrolyser performance, influencing the voltage losses (polarisation and ohmic) and stability. To mitigate issues associated with Ti PTL passivation and enhance charge transport, various noble metal coatings, have been explored. Ir coatings seems to be the optimal solution due to their stability and catalytic activity. The review highlights surface modification techniques such as physical vapour deposition, electroplating, and laser ablation, as well as the development of porous transport electrodes and microporous layers. These approaches aim to optimise the performance of the electrolyser while minimising the noble metal usage. The findings underscore the importance of material choice and nano/microscale morphology of the interface in achieving cost-effective and durable PEMWE systems.
{"title":"Interface between anode porous transport layer and catalyst layer: A key to efficient, stable and competitive proton exchange membrane water electrolysis","authors":"Tereza Bautkinova, Martin Prokop, Tomas Bystron, Karel Bouzek","doi":"10.1016/j.coelec.2024.101624","DOIUrl":"10.1016/j.coelec.2024.101624","url":null,"abstract":"<div><div>This review examines advancements in the design of the anode porous transport layer (PTL) and catalyst layer (CL) interface in proton exchange membrane water electrolysis (PEMWE). The quality of PTL-CL interface (contact area and contact resistance per area) is critical to electrolyser performance, influencing the voltage losses (polarisation and ohmic) and stability. To mitigate issues associated with Ti PTL passivation and enhance charge transport, various noble metal coatings, have been explored. Ir coatings seems to be the optimal solution due to their stability and catalytic activity. The review highlights surface modification techniques such as physical vapour deposition, electroplating, and laser ablation, as well as the development of porous transport electrodes and microporous layers. These approaches aim to optimise the performance of the electrolyser while minimising the noble metal usage. The findings underscore the importance of material choice and nano/microscale morphology of the interface in achieving cost-effective and durable PEMWE systems.</div></div>","PeriodicalId":11028,"journal":{"name":"Current Opinion in Electrochemistry","volume":"49 ","pages":"Article 101624"},"PeriodicalIF":7.9,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143103002","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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