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Electrochemical Analysis of the Electrocatalytic Reduction of 5-Hydroxymethylfurfural in Cu Electrodes 铜电极上电催化还原5-羟甲基糠醛的电化学分析
IF 3.5 4区 化学
ChemElectroChem Pub Date : 2025-05-15 DOI: 10.1002/celc.202500007
Jose Solera-Rojas, David Carvajal, Antonio Guerrero, Carmen Mejuto, Elena Mas-Marzá, Francisco Fabregat-Santiago
{"title":"Electrochemical Analysis of the Electrocatalytic Reduction of 5-Hydroxymethylfurfural in Cu Electrodes","authors":"Jose Solera-Rojas,&nbsp;David Carvajal,&nbsp;Antonio Guerrero,&nbsp;Carmen Mejuto,&nbsp;Elena Mas-Marzá,&nbsp;Francisco Fabregat-Santiago","doi":"10.1002/celc.202500007","DOIUrl":"https://doi.org/10.1002/celc.202500007","url":null,"abstract":"<p>The electroreduction of 5-hydroxymethylfurfural (HMF) offers promising opportunities for the synthesis of valuable chemical precursors. However, achieving high selectivity in this process remains challenging due to the complexity of the reaction mechanisms involved. Here, this study employs different electrochemical techniques to analyze each of the HMF electroreduction pathways. These findings demonstrate that the primary products of HMF electroreduction are 2,5-bis(hydroxymethyl)furan (BHMF) and 5-methylfurfural alcohol (MFA), with lower formation of 5-methylfurfural (5-MF) and 2,5-dimethylfuran. This study identifies a significant competition between hydrogen evolution reaction and the reduction of HMF and 5-MF that affect the faradaic efficiencies of the organic transformation. In contrast, BHMF and MFA display a reduced reactivity, behaving as terminal molecules. Through impedance analysis, it is possible to follow the reaction pathways by associating each reaction step with the changes observed in charge transfer and accumulation phenomena. These are key parameters for understanding the reaction mechanisms in the system as they allow to distinguish between adsorption, absorption and reaction of the organic molecules onto the electrode surface. This approach helps to accurately select the optimal potential for the reduction reactions. The results obtained in this study facilitate the design of efficient and selective electrocatalytic systems for biomass conversion.</p>","PeriodicalId":142,"journal":{"name":"ChemElectroChem","volume":"12 11","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/celc.202500007","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144256606","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Electrodeposition of Thermoelectric Materials 热电材料的电沉积
IF 3.5 4区 化学
ChemElectroChem Pub Date : 2025-05-15 DOI: 10.1002/celc.202500052
Samuel C. Perry, Samina Akbar, Robert Clarke, Syed Z. H. Shah, Iris Nandhakumar
{"title":"Electrodeposition of Thermoelectric Materials","authors":"Samuel C. Perry,&nbsp;Samina Akbar,&nbsp;Robert Clarke,&nbsp;Syed Z. H. Shah,&nbsp;Iris Nandhakumar","doi":"10.1002/celc.202500052","DOIUrl":"https://doi.org/10.1002/celc.202500052","url":null,"abstract":"<p>Thermoelectric (TE) materials produce electrical energy when exposed to a thermal gradient and so have unsurprisingly gathered increasing interest as a promising tool in the route to reduced carbon energy emissions. However, many synthetic routes currently involve high-temperatures, oxygen-free environments and harsh chemical reagents. Electrochemistry offers an attractive alternate synthetic route for similar materials at greatly reduced temperatures, without the need for strong chemical reductants. This review looks at recent developments in the electrodeposition of TE materials, highlighting promising materials and techniques. It also outlines key challenges that must be addressed in order to advance the readiness of this technology for wider implementation.</p>","PeriodicalId":142,"journal":{"name":"ChemElectroChem","volume":"12 15","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/celc.202500052","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144705520","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
The Role of Hexagonal Boron Nitride (h-BN) in Enhancing Electrolytes for Safer and Efficient Lithium-Based Batteries 六方氮化硼(h-BN)在增强更安全高效锂基电池电解质中的作用
IF 3.5 4区 化学
ChemElectroChem Pub Date : 2025-05-15 DOI: 10.1002/celc.202500011
Gulsah Yaman Uzunoglu, Sahin Coskun, Recep Yuksel
{"title":"The Role of Hexagonal Boron Nitride (h-BN) in Enhancing Electrolytes for Safer and Efficient Lithium-Based Batteries","authors":"Gulsah Yaman Uzunoglu,&nbsp;Sahin Coskun,&nbsp;Recep Yuksel","doi":"10.1002/celc.202500011","DOIUrl":"https://doi.org/10.1002/celc.202500011","url":null,"abstract":"<p>Hexagonal boron nitride (h-BN), with its unique structural and thermal properties, has emerged as a versatile material capable of addressing challenges such as thermal instability, dendrite formation, and limited ionic conductivity across liquid, gel polymer, and solid-state electrolytes (SSEs) for high-performing lithium ion and lithium metal batteries (LMBs). In liquid electrolytes, h-BN improves ionic mobility and suppresses side reactions, while in gel polymer electrolytes (GPEs), it enhances mechanical flexibility and thermal stability. SSEs benefit from h-BN's ability to suppress dendrites, reinforce mechanical strength, and optimize interfacial compatibility, making it a key enabler for next-generation battery technologies. Despite its promise, challenges such as dispersion uniformity, cost, and interfacial complexity must be addressed. Future directions, including the development of multifunctional architectures, dynamic electrolytes, and sustainable synthesis methods, are discussed to guide the integration of h-BN in emerging energy storage systems. This perspective article explores the multifunctional roles of h-BN, highlighting its contributions to enhancing ionic transport, thermal management, and interfacial stability. By presenting a comprehensive overview of h-BN's role in electrolytes, this work aims to inspire further research into its potential to revolutionize energy storage technologies.</p>","PeriodicalId":142,"journal":{"name":"ChemElectroChem","volume":"12 11","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/celc.202500011","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144256607","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mechanisms of Oxygen Reactions in Lithium–Air Batteries 锂-空气电池氧反应机理研究
IF 3.5 4区 化学
ChemElectroChem Pub Date : 2025-05-12 DOI: 10.1002/celc.202500051
Andrea P. Gualdron-Plata, Vivian Y. Brizola, Vitor L. Martins
{"title":"Mechanisms of Oxygen Reactions in Lithium–Air Batteries","authors":"Andrea P. Gualdron-Plata,&nbsp;Vivian Y. Brizola,&nbsp;Vitor L. Martins","doi":"10.1002/celc.202500051","DOIUrl":"https://doi.org/10.1002/celc.202500051","url":null,"abstract":"<p>The complicated O<sub>2</sub> reactions at the battery's positive electrode hinder the development of Li–air and Li–O<sub>2</sub> batteries. The oxygen reduction reaction (during battery discharge) and the oxygen evolution reaction (during battery charge) are still not fully elucidated, and more than one mechanism has been proposed for each process. These mechanisms greatly depend on the electrolyte's physicochemical properties, which opens the possibility of favoring a more desired one. Nonetheless, recent findings have shown that this is not always the case. Therefore, this perspective aims to provide a brief overview of the current understanding of the most widely accepted mechanisms and discuss the impact of the most recent findings.</p>","PeriodicalId":142,"journal":{"name":"ChemElectroChem","volume":"12 12","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/celc.202500051","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144256542","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Tracing Iridium Dissolution Pathways in Proton Exchange Membrane Water Electrolyzers at Relevant Current Densities in Real Time 实时追踪相关电流密度下质子交换膜水电解槽中铱的溶解途径
IF 3.5 4区 化学
ChemElectroChem Pub Date : 2025-05-12 DOI: 10.1002/celc.202500098
Nico C. Röttcher, Jiahua Zhou, Lukas Löttert, Karl J. J. Mayrhofer, Dominik Dworschak
{"title":"Tracing Iridium Dissolution Pathways in Proton Exchange Membrane Water Electrolyzers at Relevant Current Densities in Real Time","authors":"Nico C. Röttcher,&nbsp;Jiahua Zhou,&nbsp;Lukas Löttert,&nbsp;Karl J. J. Mayrhofer,&nbsp;Dominik Dworschak","doi":"10.1002/celc.202500098","DOIUrl":"https://doi.org/10.1002/celc.202500098","url":null,"abstract":"<p>Catalyst dissolution is one of the key challenges in achieving long-term performance in proton exchange membrane water electrolysis with low iridium loading. However, most of the dissolved catalyst remains in the catalyst-coated membrane, inaccessible for operando quantification. While simpler aqueous model systems improve mechanistic understanding, dissolution rates are significantly overestimated compared to the device level. To bridge this gap, herein, an electrochemical half-cell setup that mimics the anode catalyst layer environment to enable operation at relevant current densities (&gt;1 <span></span><math></math>) is presented. Dissolved catalyst species transported through the porous transport layer or through the membrane are separately detected operando by coupling to inductively coupled plasma-mass spectrometry. The results demonstrate a strong preference for the transport of dissolved iridium through the membrane (99.9%) and a decrease in catalyst stability by factor 10 at high current densities. Discrepancies with so far reported findings from full-cell and half-cell experiments highlight a lack of understanding of catalyst dissolution and the transportation of dissolved species in different systems. The presented method offers unique insights which will help to study and optimize catalyst dissolution by means of various manufacturing and operation parameters to ultimately improve the stability of catalyst layers for water electrolysis.</p>","PeriodicalId":142,"journal":{"name":"ChemElectroChem","volume":"12 15","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/celc.202500098","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144705305","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Ten-Membered Cyclic Azobenzene: Electrochemical Synthesis and Photochromic Properties 十元环偶氮苯的电化学合成及其光致变色性能
IF 3.5 4区 化学
ChemElectroChem Pub Date : 2025-05-12 DOI: 10.1002/celc.202500111
Qianqian Niu, Dan Li, Lijiao Guo, Xinyuan Sun, Yan Liu, Longjiu Cheng, Baokang Jin
{"title":"Ten-Membered Cyclic Azobenzene: Electrochemical Synthesis and Photochromic Properties","authors":"Qianqian Niu,&nbsp;Dan Li,&nbsp;Lijiao Guo,&nbsp;Xinyuan Sun,&nbsp;Yan Liu,&nbsp;Longjiu Cheng,&nbsp;Baokang Jin","doi":"10.1002/celc.202500111","DOIUrl":"https://doi.org/10.1002/celc.202500111","url":null,"abstract":"<p>Cyclic azobenzenes generally exhibit enhanced photophysical properties compared to conventional linear azobenzenes, such as visible-light activation and exceptional thermal stability. However, their broader application has been hindered by synthetic challenges. Herein, the electrochemical synthesis of a ten-membered cyclic azobenzene, 6,7-dihydrodibenzo[e,i][1,4,7,8]dioxadiazecine (DDEI), is reported through the reduction of 1,2-bis(2-nitrophenoxy)ethane (BNPOE) in the presence of CO<sub>2</sub>. The reduction mechanism, involving an irreversible eight-electron process and CO<sub>2</sub> capture, is elucidated using in situ fourier transform infrared spectroscopy (FT-IR) spectroelectrochemistry, complemented by <sup>13</sup>C NMR, <sup>1</sup>H NMR, and mass spectrometry analyzes. Both experimental results and density functional theory calculations show that DDEI undergoes highly efficient <i>trans</i>-to-<i>cis</i> isomerization under green light (500 nm) irradiation, achieving a remarkable yield of 97%, with both isomers exhibiting excellent thermal stability. In contrast to 8- and 9-membered cyclic azobenzenes and in line with conventional linear azobenzenes, the <i>trans</i> configuration of DDEI is more stable than the <i>cis</i> configuration. This combination of synthetic accessibility and superior photophysical properties makes DDEI a promising candidate for various applications, including those in living systems.</p>","PeriodicalId":142,"journal":{"name":"ChemElectroChem","volume":"12 15","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/celc.202500111","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144705607","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Investigating the Fuel Cell Performance Tradeoffs of Thick Catalyst Layers 研究厚催化剂层对燃料电池性能的影响
IF 3.5 4区 化学
ChemElectroChem Pub Date : 2025-05-12 DOI: 10.1002/celc.202500038
Rifael Z. Snitkoff-Sol, Yan Presman, Lior Elbaz
{"title":"Investigating the Fuel Cell Performance Tradeoffs of Thick Catalyst Layers","authors":"Rifael Z. Snitkoff-Sol,&nbsp;Yan Presman,&nbsp;Lior Elbaz","doi":"10.1002/celc.202500038","DOIUrl":"https://doi.org/10.1002/celc.202500038","url":null,"abstract":"<p>Platinum group metal-free (PGM-free) catalysts are showing increasing performance and durability and are considered as viable candidates for replacing precious metal-based catalysts for the oxygen reduction reaction (ORR) in fuel cells. Due to the low intrinsic activity and low active site density, large quantities of the PGM-free catalysts are needed to obtain high performance. Consequently, the resulting high catalyst loadings induce several interesting and opposing phenomena, namely, lower ORR kinetic losses due to an increase in the number of active sites and much higher mass and charge transport losses. In this work, Fourier-transformed alternating current voltammetry (FTacV) and electrochemical impedance spectroscopy (EIS) measurements are employed to systematically deconvolute the gains and losses to the activity due to the high loading of PGM-free catalysts and relate the underlying processes to the observed fuel cell performance. EIS is analyzed via extraction of the distribution of relaxation times, obtaining a model-free analysis of the physical processes in the cell. Combined with FTacV measurements, the obtained catalyst loading optimum from a mechanistic point of view is explained. The combined use of advanced alternating current techniques for the analysis of operating fuel cells is an important step toward the rational design of the catalyst layer.</p>","PeriodicalId":142,"journal":{"name":"ChemElectroChem","volume":"12 10","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/celc.202500038","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144131510","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A Reexamination of CO2 Reduction with Fe2S2 Hydrogenase Mimics: Lessons in Using a Hydrogen Evolution Reaction Catalyst for CO2 to Formate Catalysis Fe2S2氢化酶模拟物对CO2还原的再考察:用析氢反应催化剂催化CO2生成甲酸的经验教训
IF 3.5 4区 化学
ChemElectroChem Pub Date : 2025-05-12 DOI: 10.1002/celc.202500030
Christopher J. Miller, Byunghoon Lee, Jacob A. Barrett, Joseph M. Palasz, Thomas Chan, Anoushka Shandilya, Clifford P. Kubiak
{"title":"A Reexamination of CO2 Reduction with Fe2S2 Hydrogenase Mimics: Lessons in Using a Hydrogen Evolution Reaction Catalyst for CO2 to Formate Catalysis","authors":"Christopher J. Miller,&nbsp;Byunghoon Lee,&nbsp;Jacob A. Barrett,&nbsp;Joseph M. Palasz,&nbsp;Thomas Chan,&nbsp;Anoushka Shandilya,&nbsp;Clifford P. Kubiak","doi":"10.1002/celc.202500030","DOIUrl":"https://doi.org/10.1002/celc.202500030","url":null,"abstract":"<p>Recent reports show [FeFe] hydrogenase mimics are active for the electrochemical reduction of CO<sub>2</sub> to formate (HCOO<sup>−</sup>). Herein, the electrochemical reduction of CO<sub>2</sub> with the [FeFe] hydrogenase mimic [Fe<sub>2</sub>(μ-pdt)(CO)<sub>6</sub>, <b>1</b>, where pdt = propane-1,3-dithiolate] in acetonitrile is reported. In the presence of the weak acid, methanol (MeOH), <b>1</b> reduces CO<sub>2</sub> to both CO (Faradaic Efficiency maximum [FE<sub>max</sub>] of 16 ± 6%) and HCOO<sup>−</sup> (FE<sub>max</sub> = 20%) and produces H<sub>2</sub> (FE<sub>max</sub> = 56 ± 4%). Without added MeOH, <b>1</b> reacts with adventitious water to form H<sub>2</sub> (FE<sub>max</sub> = 85 ± 1%), HCOO<sup>−</sup> (FE<sub>max</sub> = 7.8%), and CO (FE<sub>max</sub> = 7 ± 3%) with CO<sub>3</sub><sup>2−</sup> being detected by infrared spectroscopy.  Product formation is potential dependent: more negative potentials increases selectivity for HCOO<sup>−</sup> over CO. The first reduction of <b>1</b> forms a pdt-bridged dimer, <b>2</b>. However, the reduction of <b>2</b> at the potentials required for electrochemical CO<sub>2</sub> reduction leads to two new species. Using density functional theory, and infrared spectroelectrochemistry (IR-SEC), these structures are identified to be [Fe(CO)<sub>4</sub>]<sup>2−</sup> (<b>3</b>) and a trinuclear Fe<sub>3</sub> species (<b>4</b>). While these species can reduce CO<sub>2</sub> to CO and HCOO<sup>−</sup>, the predominant formation of H<sub>2</sub> reveals kinetic issues in  CO<sub>2</sub> reduction. The work offers to consider alternate competing mechanistic pathways and explains the lack of product selectivity when using hydrogen evolution reaction catalyst for CO<sub>2</sub> reduction to HCOO<sup>−</sup>.</p>","PeriodicalId":142,"journal":{"name":"ChemElectroChem","volume":"12 13","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/celc.202500030","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144551232","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Enhanced Alkaline Water Electrolysis with PrBa0.5Sr0.5Co1.5Fe0.5O5+δ-IrO2 Composite: Synergistic Catalytic Performance via Electronic Structure Modulation PrBa0.5Sr0.5Co1.5Fe0.5O5+δ-IrO2复合材料增强碱性水电解:电子结构调制的协同催化性能
IF 3.5 4区 化学
ChemElectroChem Pub Date : 2025-05-08 DOI: 10.1002/celc.202500031
Zixuan Fan, Yaowei Liu, Jianqiang Wang, Lakshya Mathur, Sivaprakash Sengodan, Bingbing Niu, Guntae Kim
{"title":"Enhanced Alkaline Water Electrolysis with PrBa0.5Sr0.5Co1.5Fe0.5O5+δ-IrO2 Composite: Synergistic Catalytic Performance via Electronic Structure Modulation","authors":"Zixuan Fan,&nbsp;Yaowei Liu,&nbsp;Jianqiang Wang,&nbsp;Lakshya Mathur,&nbsp;Sivaprakash Sengodan,&nbsp;Bingbing Niu,&nbsp;Guntae Kim","doi":"10.1002/celc.202500031","DOIUrl":"https://doi.org/10.1002/celc.202500031","url":null,"abstract":"<p><i>Alkaline water electrolysis</i> (AWS) is a promising technology for hydrogen production, but the low performance of oxygen evolution reaction (OER) electrodes leads to high energy consumption. Enhancing OER efficiency is essential for reducing energy barriers and improving system performance. In this study, it develops a composite catalyst of PrBa<sub>0.5</sub>Sr<sub>0.5</sub>Co<sub>1.5</sub>Fe<sub>0.5</sub>O<sub>5+δ</sub> and IrO<sub>2</sub> (PBSCF-Ir), with a surface area of 18.68 m<sup>2</sup>g<sup>−1</sup>. The PBSCF-Ir composite exhibits a low overpotential of 312 mV at 10 mA cm<sup>−2</sup> and stability over 300 h. In water splitting tests, it achieves a lower cell voltage (1.95 V at 500 mA cm<sup>−2</sup>) compared to pure IrO<sub>2</sub>. X-ray photoelectron spectroscopy reveals a 1 eV blueshift in Co 2p energy levels, indicating modified electronic structures. Density functional theory calculations show that IrO<sub>2</sub> shifts the d-band centers of Co and Fe, enhancing electrophilicity, OH<sup>−</sup> affinity, and OER activity. This study highlights the PBSCF-Ir composite as an efficient and durable catalyst for AWS, thereby addressing the need for sustainable hydrogen production.</p>","PeriodicalId":142,"journal":{"name":"ChemElectroChem","volume":"12 12","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/celc.202500031","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144255888","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Tetraethylammonium Cation Activates Fe for Selective Electroreduction of CO2 to Oxalate 四乙基铵阳离子活化铁选择性电还原CO2为草酸盐
IF 3.5 4区 化学
ChemElectroChem Pub Date : 2025-05-08 DOI: 10.1002/celc.202500093
Rohan Sartape, Rohit Chauhan, Venkata S. R. P. Yadavalli, Ishita Goyal, Ishaku Amos, Yancun Qi, Vamsi V. Gande, Abdul M. Sarkar, Ksenija D. Glusac, Meenesh R. Singh
{"title":"Tetraethylammonium Cation Activates Fe for Selective Electroreduction of CO2 to Oxalate","authors":"Rohan Sartape,&nbsp;Rohit Chauhan,&nbsp;Venkata S. R. P. Yadavalli,&nbsp;Ishita Goyal,&nbsp;Ishaku Amos,&nbsp;Yancun Qi,&nbsp;Vamsi V. Gande,&nbsp;Abdul M. Sarkar,&nbsp;Ksenija D. Glusac,&nbsp;Meenesh R. Singh","doi":"10.1002/celc.202500093","DOIUrl":"https://doi.org/10.1002/celc.202500093","url":null,"abstract":"<p>The strong binding energy of CO on iron surfaces has rendered Fe electrodes as poor electrochemical CO<sub>2</sub> reduction (eCO2R) catalysts, predominantly producing hydrogen. Recent studies on tuning the microenvironment near the catalyst surfaces by tuning the local electric field in nonaqueous environments have been shown to promote eCO2R by facilitating the CO<sub>2</sub> activation step. Herein, the use of tetraethylammonium (TEA) cation to tune the electric field on Fe surfaces, such that it leads to the formation of industrially relevant oxalates (C<sub>2</sub> products), is reported. At optimal cation concentrations, the developed eCO2R system achieves 25 mA cm<sup>−2</sup> of current density and Faradaic Efficiencies up to 75% toward oxalate. Furthermore, in situ attenuated total reflectance Fourier transform infrared spectroscopy indicates the presence of surface-adsorbed TEA cations and other species on the Fe surfaces, leading to the well-known outer-sphere mechanism of electron transfer during eCO2R. The employment of Fe, along with microenvironment tuning, not only demonstrates high catalytic performance but also provides a safer and more sustainable alternative to toxic catalysts such as Pb that dominate the nonaqueous eCO<sub>2</sub>R literature. These findings pave the way for further optimization and scale-up of the process, offering a viable route for sustainable chemical production and CO<sub>2</sub> mitigation.</p>","PeriodicalId":142,"journal":{"name":"ChemElectroChem","volume":"12 15","pages":""},"PeriodicalIF":3.5,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/celc.202500093","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144705338","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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