EES catalysis最新文献

筛选
英文 中文
Advances in catalysing the hydrogen storage in main group metals and their tetrahydroborates and tetrahydroaluminates 主族金属及其四氢硼酸盐和四氢铝酸盐储氢催化研究进展
EES catalysis Pub Date : 2025-07-23 DOI: 10.1039/D5EY00134J
Melinda Krebsz, Tibor Pasinszki, Sooraj Sreenath and Valeska P. Ting
{"title":"Advances in catalysing the hydrogen storage in main group metals and their tetrahydroborates and tetrahydroaluminates","authors":"Melinda Krebsz, Tibor Pasinszki, Sooraj Sreenath and Valeska P. Ting","doi":"10.1039/D5EY00134J","DOIUrl":"https://doi.org/10.1039/D5EY00134J","url":null,"abstract":"<p >Hydrogen is a promising clean and renewable energy source; however, its efficient storage is one of the key challenges in establishing the sustainable hydrogen economy. The light main group metals and their tetrahydroborates and tetrahydroaluminates show great potential for high hydrogen storage capacity close to ambient conditions; however, their high hydrogenation and dehydrogenation temperatures, sluggish kinetics, and limited reversibility have always been an obstacle for practical applications. Large efforts have been devoted to modifying the thermodynamic and kinetic properties of these systems, and reviewing these efforts and highlighting future directions are the aims of the present review. Based on recent research, the application of multicomponent systems utilizing multiple modification methods, such as catalysis, nanoconfinement, alloying, and structure engineering, is essential for enhancing the storage conditions. The synergistic effect of multiple catalysts is now a key requirement to address various steps of the overall process, including forming/breaking the H–H and metal–H bonds, transporting hydrogen and heat, and suppressing the formation of side products. Compared to pristine systems, tremendous improvement has been achieved. Catalysed AlH<small><sub>3</sub></small> decomposition can now operate as a one-way hydrogen source below 100 °C and the Mg/MgH<small><sub>2</sub></small> hydrogen storage system exhibits good cyclic performance at elevated temperatures. Metal hydrides, tetrahydroborates, tetrahydroaluminates, and their composite systems face challenges in achieving close to ambient operating conditions and cyclic stability. As the demand for improved hydrogen energy storage is expected to grow, further research for the enhancement of these systems will continue to advance the state of hydrogen storage technology.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 6","pages":" 1196-1228"},"PeriodicalIF":0.0,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00134j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145429071","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
Dynamic evolution of self-renewal Fe–N–C catalysts for the acidic oxygen reduction reaction† 自更新Fe-N-C催化剂在酸性氧还原反应中的动态演化
EES catalysis Pub Date : 2025-07-22 DOI: 10.1039/D5EY00092K
Fangzhou Liu, Leo Lai, Zhongyuan Guo, Fangxin She, Justin Prabowo, Hao Li, Li Wei and Yuan Chen
{"title":"Dynamic evolution of self-renewal Fe–N–C catalysts for the acidic oxygen reduction reaction†","authors":"Fangzhou Liu, Leo Lai, Zhongyuan Guo, Fangxin She, Justin Prabowo, Hao Li, Li Wei and Yuan Chen","doi":"10.1039/D5EY00092K","DOIUrl":"https://doi.org/10.1039/D5EY00092K","url":null,"abstract":"<p >Heterogeneous molecular Fe–N–C catalysts hold promise for the oxygen reduction reaction (ORR), but their stability in acidic media remains a bottleneck. Here, we report the synthesis of a self-renewal Fe–N–C catalyst by uniformly polymerizing an iron polyphthalocyanine (FePPc) shell around carbon nanotubes (CNTs) <em>via</em> a microwave-assisted method. This FePPc/CNT catalyst achieves a much higher Fe mass loading (2.92 wt%) compared to directly depositing iron phthalocyanine (FePc) molecules on CNTs (FePc/CNT, 0.80 wt%) while maintaining a similar density of exposed Fe–N<small><sub>4</sub></small> sites to electrolytes. FePPc/CNT exhibits superior ORR activity in 0.1 M HClO<small><sub>4</sub></small> electrolyte with a half-wave potential (<em>E</em><small><sub>1/2</sub></small>) of 0.74 V (<em>vs.</em> reversible hydrogen electrode), a low Tafel slope of 51 mV dec<small><sup>−1</sup></small>, and a high turnover frequency (TOF) of 0.98 site<small><sup>−1</sup></small> s<small><sup>−1</sup></small>. Density functional theory (DFT) calculations attribute this enhanced activity to strong FePPc–CNT interactions that facilitate efficient electron transfer and favorable reaction energetics. Critically, FePPc/CNT demonstrates enhanced stability in the acidic electrolyte, retaining ∼80% of its initial current density after 24 h of the chronoamperometric test, outperforming FePc/CNT (42% after 5 h) and physically mixed FePPc and CNTs (49% after 24 h). Quantitative analysis reveals a unique self-renewal mechanism involving layer-by-layer shedding of FePPc, which exposes fresh active sites to sustain catalytic activity. At the same time, detached FePPc fragments sediment on CNTs. Furthermore, leached Fe ions migrate onto CNTs and aggregate into FeO<small><sub><em>x</em></sub></small> nanoclusters, eventually leading to irreversible deactivation. These findings provide new insights for designing durable Fe–N–C catalysts for various reactions.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 6","pages":" 1358-1368"},"PeriodicalIF":0.0,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00092k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145429070","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
Stabilizing amorphous NiFe-based catalysts via borate bridging for water oxidation under industrial conditions† 工业条件下硼酸桥接稳定非晶镍铁基催化剂的水氧化作用
EES catalysis Pub Date : 2025-07-22 DOI: 10.1039/D5EY00157A
Wei Qi, Youze Zeng, Liuqing Wang, Jinsheng Li, Zhuoqi Wang, Feiyan An, Kai Li, Meiling Xiao, Changpeng Liu, Wei Xing and Jianbing Zhu
{"title":"Stabilizing amorphous NiFe-based catalysts via borate bridging for water oxidation under industrial conditions†","authors":"Wei Qi, Youze Zeng, Liuqing Wang, Jinsheng Li, Zhuoqi Wang, Feiyan An, Kai Li, Meiling Xiao, Changpeng Liu, Wei Xing and Jianbing Zhu","doi":"10.1039/D5EY00157A","DOIUrl":"https://doi.org/10.1039/D5EY00157A","url":null,"abstract":"<p >The practical deployment of an anion exchange membrane water electrolyzer (AEMWE) relies on the exploration of active and durable electrocatalysts towards the sluggish oxygen evolution reaction (OER). Although amorphous NiFe-based catalysts (a-NiFeO<small><sub><em>x</em></sub></small>H<small><sub><em>y</em></sub></small>) emerge as the competitive candidate due to impressive intrinsic OER activity, their unique defective structure renders the metal sites more susceptible to over-oxidation and dissolution, leading to poor stability. To address this challenge, we incorporate borate groups (BO<small><sub>3</sub></small><small><sup>3−</sup></small>) into the a-NiFeO<small><sub><em>x</em></sub></small>H<small><sub><em>y</em></sub></small> lattice by occupying the oxygen vacancy sites. The bridged borates not only maintain the structural stability <em>via</em> filling the oxygen vacancies, but also assist electron transfer from Ni to Fe to suppress Fe ion dissolution, thereby enhancing the catalytic stability of a-NiFeO<small><sub><em>x</em></sub></small>H<small><sub><em>y</em></sub></small>. Moreover, the tailored electronic structure of Ni favors electrochemical reconstruction to high-valence Ni active species and optimizes adsorption of oxygen intermediates towards superior OER activity. Therefore, a-B-NiFeO<small><sub><em>x</em></sub></small>H<small><sub><em>y</em></sub></small> integrated into the AEMWE can deliver a noteworthy current density of 4.75 A cm<small><sup>−2</sup></small> at a voltage of 2.0 V and maintain stable operation at 0.5 A cm<small><sup>−2</sup></small> for 3000 hours. This study not only affords a promising electrocatalyst for the AEMWE, but also paves a new avenue to break the activity-stability trade-off of amorphous materials for the OER.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 6","pages":" 1369-1376"},"PeriodicalIF":0.0,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00157a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145429075","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
How the electric double layer impacts nitrate reduction to ammonia† 双电层如何影响硝酸盐还原为氨†
EES catalysis Pub Date : 2025-07-21 DOI: 10.1039/D5EY00217F
Sofia Czerny-Holownia, Hailey R. Boyer, Alex J. King, Victoria Y. Yang, Jinyu Guo, Matthew J. Liu, Justin C. Bui, William A. Tarpeh and Eric W. Lees
{"title":"How the electric double layer impacts nitrate reduction to ammonia†","authors":"Sofia Czerny-Holownia, Hailey R. Boyer, Alex J. King, Victoria Y. Yang, Jinyu Guo, Matthew J. Liu, Justin C. Bui, William A. Tarpeh and Eric W. Lees","doi":"10.1039/D5EY00217F","DOIUrl":"https://doi.org/10.1039/D5EY00217F","url":null,"abstract":"<p >Electrochemical nitrate reduction (ENR) is an appealing method for remediating nitrate contamination in wastewater and producing ammonia using renewable electricity. However, a mechanistic understanding of coupled mass transfer and electrocatalysis at the electrode–electrolyte interface, which dictates ENR efficiency, is limited. In this study, we develop an experimentally-validated multiphysics model of the Stern, diffuse, and diffusion layers near the surface of a polycrystalline titanium catalyst to investigate the effect of the electric double layer on ENR. The developed model couples the generalized-modified-Nernst–Planck equation with Frumkin–Butler–Volmer kinetics and numerical optimization to quantify the effect of applied potential and bulk electrolyte concentration on the ammonia formation rate. Our results reveal how dynamic driving forces at the polarized interface give rise to experimentally observed trends in ENR. Guided by this insight, we show that a more negative potential-of-zero-charge increases the limiting current density for ammonia synthesis by enabling faster migration of nitrate towards the cathode surface. The results motivate the development of multi-scale models that link transport phenomena with molecular-scale modelling to design and tailor interfaces for efficient ENR.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 6","pages":" 1272-1284"},"PeriodicalIF":0.0,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00217f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145429050","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
Carbon-supported platinum-based electrocatalysts for alkaline hydrogen evolution 碳负载铂基碱性析氢电催化剂
EES catalysis Pub Date : 2025-07-18 DOI: 10.1039/D5EY00147A
Qiuyue Yang, Jilan Zeng, Guowei Yang, Xinran Sun, Xiahui Lin, Kunlong Liu, Jiayi Chen, Sibo Wang and Xue Feng Lu
{"title":"Carbon-supported platinum-based electrocatalysts for alkaline hydrogen evolution","authors":"Qiuyue Yang, Jilan Zeng, Guowei Yang, Xinran Sun, Xiahui Lin, Kunlong Liu, Jiayi Chen, Sibo Wang and Xue Feng Lu","doi":"10.1039/D5EY00147A","DOIUrl":"https://doi.org/10.1039/D5EY00147A","url":null,"abstract":"<p >Water electrolysis hydrogen production technology directly generates high-purity hydrogen through electrochemical water splitting, serving as a key technology for achieving zero-carbon emission hydrogen production. Alkaline water electrolysis demonstrates marked advantages in efficiency and rapidly developing anode catalysts in an alkaline medium. Nevertheless, the sluggish kinetics of the hydrogen evolution reaction (HER) at the cathode in an alkaline environment constitute a fundamental bottleneck that restricts the extensive application of this technology. Platinum, serving as the benchmark catalyst for the HER, is limited in its large-scale development due to its scarcity and high cost. In comparison, carbon-supported platinum-based catalysts exhibit exceptional HER catalytic activity and stability, driven by their unique electronic architecture and the synergistic effect with the support. In this review, we comprehensively examine the latest progress of carbon-supported platinum-based materials for the alkaline HER, summarize the factors contributing to the slow kinetics of the HER in an alkaline environment, and then focus on the strategies for modifying the carbon substrate and synthesizing carbon-supported platinum-based nanomaterials. Finally, the review critically evaluates existing challenges and proposes targeted research directions to advance Pt-based electrocatalysts for practical alkaline hydrogen evolution systems.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 972-993"},"PeriodicalIF":0.0,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00147a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990362","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
Optimization of competitive adsorption via oxygen vacancies on NiCo hydroxides for selective electrosynthesis of adipic acid coupled with hydrogen production† 选择性电合成己二酸产氢过程中NiCo羟基氧空位竞争吸附的优化
EES catalysis Pub Date : 2025-07-17 DOI: 10.1039/D5EY00137D
Xun Pan, Lingzhi Sun, Kuang Chen, Jingui Zheng, Shaohan Xu, Chao Miao and Guohua Zhao
{"title":"Optimization of competitive adsorption via oxygen vacancies on NiCo hydroxides for selective electrosynthesis of adipic acid coupled with hydrogen production†","authors":"Xun Pan, Lingzhi Sun, Kuang Chen, Jingui Zheng, Shaohan Xu, Chao Miao and Guohua Zhao","doi":"10.1039/D5EY00137D","DOIUrl":"https://doi.org/10.1039/D5EY00137D","url":null,"abstract":"<p >The electrosynthesis of adipic acid through the cyclohexanol oxidation reaction (COR) can address the pollution issues associated with the traditional process. However, the complexity of the electrooxidation process and unclear dehydrogenation and oxidation mechanisms limit its application. Herein, we report oxygen vacancy (V<small><sub>O</sub></small>) modification on NiCo hydroxides for the selective electrosynthesis of adipic acid. <em>In situ</em> IR and DFT calculations revealed significantly enhanced adsorption capacity and an optimized process for the co-adsorption of OH<small><sup>−</sup></small> and organic compounds. The V<small><sub>O</sub></small> promotes the conversion of ketone intermediates into glycol with the addition of H<small><sub>2</sub></small>O while inhibiting the formation of ketone alcohols. <em>In situ</em> synchrotron radiation and Raman analyses reveal the reversible remodeling processes of Ni<small><sup>2+</sup></small>–OH and Ni<small><sup>3+</sup></small>–OOH during the COR. Consequently, V<small><sub>O</sub></small>-NiCo demonstrated excellent COR performance (1.32 V <em>vs.</em> RHE onset potential) with conversion, adipic acid selectivity, and faradaic efficiency values of 98.4%, 95.6%, and 95.2%, respectively. The system generates 8.2 times more hydrogen compared with pure water splitting at the cathode. This integrated electrocatalytic system shows potential for large-scale production of H<small><sub>2</sub></small> and adipic acid, offering new insights for designing advanced electrocatalysts for cost-effective and sustainable energy conversion.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 6","pages":" 1345-1357"},"PeriodicalIF":0.0,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00137d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145429056","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
Plasma-driven redox mechanism in the reverse water–gas shift reaction over Ni–In intermetallic catalysts† Ni-In金属间催化剂上逆水气转换反应的等离子体驱动氧化还原机制
EES catalysis Pub Date : 2025-07-17 DOI: 10.1039/D5EY00101C
Dae-Yeong Kim, Zhang Wenjun, Kaiyue Dong, Bang Lu, Duanxing Li, Satoru Takakusagi, Shinya Furukawa and Tomohiro Nozaki
{"title":"Plasma-driven redox mechanism in the reverse water–gas shift reaction over Ni–In intermetallic catalysts†","authors":"Dae-Yeong Kim, Zhang Wenjun, Kaiyue Dong, Bang Lu, Duanxing Li, Satoru Takakusagi, Shinya Furukawa and Tomohiro Nozaki","doi":"10.1039/D5EY00101C","DOIUrl":"https://doi.org/10.1039/D5EY00101C","url":null,"abstract":"<p >The reverse water–gas shift (RWGS) reaction has been recognized as a promising strategy for CO<small><sub>2</sub></small> valorization. However, it faces limitations due to low activity and poor CO selectivity at low temperatures. In this study, we report that plasma can effectively promote the low-temperature RWGS reaction over Ni–In intermetallic catalysts. The formation of the Ni–In intermetallic phases completely suppresses CH<small><sub>4</sub></small> formation and achieves 100% CO selectivity. Through <em>in situ</em> transmission infrared spectroscopy (TIR) and <em>in situ</em> X-ray absorption fine-structure (XAFS) analysis, we monitored the changes occurring on the catalyst surface during the plasma reaction. The interaction between redox-active sites present in the Ni–In intermetallic catalysts and plasma-activated species lowers the activation energy, thereby facilitating the RWGS reaction at low temperatures. This study offers fundamental insights into how plasma-activated species enhance catalysis and the underlying mechanisms of low-temperature activation in plasma catalysis.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 1098-1105"},"PeriodicalIF":0.0,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00101c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990341","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
Vibrational excitation in plasma catalysis: how important are dynamical effects?† 等离子体催化中的振动激发:动力学效应有多重要?__
EES catalysis Pub Date : 2025-07-11 DOI: 10.1039/D5EY00132C
Floris van den Bosch, Nick Gerrits and Jörg Meyer
{"title":"Vibrational excitation in plasma catalysis: how important are dynamical effects?†","authors":"Floris van den Bosch, Nick Gerrits and Jörg Meyer","doi":"10.1039/D5EY00132C","DOIUrl":"https://doi.org/10.1039/D5EY00132C","url":null,"abstract":"<p >Plasma catalysis offers a promising alternative to current ammonia production processes, due to the combination of high selectivity of heterogenous catalysis and efficient activation of nitrogen in the plasma. However, the theoretical understanding of how various plasma processes contribute to efficiency improvements remains limited. The pioneering work of Metha <em>et al.</em> (<em>Nat. Catal.</em>, 2018, <strong>1</strong>, 269) extended the standard formulation of transition state theory by making it vibrational state-specific through the use of the Fridman–Macheret <em>α</em> model. The resulting microkinetic model accounted for vibrational contributions under the non-equilibrium conditions of a plasma reactor. In this work, we critically examine the prototypical chemical process of activated N<small><sub>2</sub></small> reactivity on ruthenium through explicit rate coefficient calculations using state-of-the-art molecular dynamics, based on a potential energy surface previously validated against molecular beam experiments. Our findings reveal that vibrational activation is significantly more effective in promoting surface reactivity than predicted by the Fridman–Macheret <em>α</em> model, which fails to capture the full complexity of state-specific contributions. Furthermore, our calculations indicate that vibrational activation is also the primary driver of highly activated thermal catalytic reactions. These results provide a valuable benchmark to guide the development of future state-specific microkinetic models for heterogeneous and plasma catalysis.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 6","pages":" 1257-1271"},"PeriodicalIF":0.0,"publicationDate":"2025-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00132c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145429049","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
Alkali-cation-free electrochemical CO2 reduction to multicarbon products in aqueous electrolytes containing tetraalkylammonium cations† 含四烷基铵阳离子的水溶液中无碱阳离子电化学CO2还原多碳产物
EES catalysis Pub Date : 2025-07-04 DOI: 10.1039/D5EY00141B
Ryo Kurihara, Shotaro Ito, Shintaro Kato, Takashi Harada, Shuji Nakanishi and Kazuhide Kamiya
{"title":"Alkali-cation-free electrochemical CO2 reduction to multicarbon products in aqueous electrolytes containing tetraalkylammonium cations†","authors":"Ryo Kurihara, Shotaro Ito, Shintaro Kato, Takashi Harada, Shuji Nakanishi and Kazuhide Kamiya","doi":"10.1039/D5EY00141B","DOIUrl":"https://doi.org/10.1039/D5EY00141B","url":null,"abstract":"<p >The electrochemical reduction of CO<small><sub>2</sub></small> to multicarbon (C<small><sub>2+</sub></small>) products is attracting attention for the sustainable production of fuel and chemicals. Conventionally, electrolytes containing alkali cations are typically used; however, salt precipitation associated with these cations often hinders stable CO<small><sub>2</sub></small> electrolysis. Organic cations are promising alternatives to alkali cations. Herein, we conducted gaseous CO<small><sub>2</sub></small> electrolysis in aqueous solutions containing tetraalkylammonium cations in the absence of alkali cations to evaluate the effect of organic cations on C<small><sub>2+</sub></small> formation. When tetramethylammonium cations were present as the only cation species besides protons, the faradaic efficiency for CO<small><sub>2</sub></small> reduction exceeded 89% across a broad current density range of 0.1–1 A cm<small><sup>−2</sup></small>. In particular, C<small><sub>2+</sub></small> formation was efficient under high total current density conditions, reaching a faradaic efficiency of 69.6% and a partial current density of 0.7 A cm<small><sup>−2</sup></small>. By contrast, the use of larger cations such as tetraethylammonium and tetrapropylammonium cations resulted in lower ethylene selectivity. Numerical simulations based on the generalized modified Poisson–Nernst–Planck model suggested that the size of the tetraalkylammonium cations affects the electric field strength within the electric double layer, with smaller cations forming a stronger field that promotes ethylene formation.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 1055-1061"},"PeriodicalIF":0.0,"publicationDate":"2025-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00141b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990337","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
Unlocking the potential: key roles of interfacial water in electrocatalysis 释放潜力:界面水在电催化中的关键作用
EES catalysis Pub Date : 2025-07-01 DOI: 10.1039/D5EY00161G
Zheng Tang, Zhongliang Dong, Lingjie Yuan, Bowen Li and Yinlong Zhu
{"title":"Unlocking the potential: key roles of interfacial water in electrocatalysis","authors":"Zheng Tang, Zhongliang Dong, Lingjie Yuan, Bowen Li and Yinlong Zhu","doi":"10.1039/D5EY00161G","DOIUrl":"https://doi.org/10.1039/D5EY00161G","url":null,"abstract":"<p >Interfacial water, serving as a subtle yet powerful performance modulator, plays a pivotal role in various electrochemical technologies due to its unique configurations and dynamic properties. Especially in the past decade, advances in electrocatalyst research, experimental characterization and theoretical modeling have significantly deepened the understanding of interfacial water's role in electrocatalytic systems. These as-obtained insights not only elucidate the dynamic behavior and structural properties of interfacial water but also highlight its importance in optimizing reaction pathways and improving electrocatalytic performance. Therefore, the understanding and regulation of interfacial water is an important topic in electrocatalytic research, and motivated us to compile this review. This review starts with a thorough analysis of interfacial water's properties and behaviors relevant to the electrocatalysis including structural types, water networks, rigidity and molecular orientation. Then, the specific roles of interfacial water in electrocatalysis are subsequently analyzed and classified as a co-catalyst, a masking agent, a regulator of reaction intermediates, and an inducer of catalyst reconfiguration. Next, some advanced experimental characterization and computational methods are presented to collectively probe the interfacial water, which is critical to capture accurate structural information. Furthermore, we present a comprehensive overview of key strategies for modulating the properties and behaviors of interfacial water to enhance the electrocatalytic performance of representative reactions at the electrolyte and catalyst levels, with emphasis on the specific mechanisms behind these modulation approaches. Finally, we discuss current challenges and future opportunities in this field, aiming to inspire the design of more advanced electrocatalytic systems.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 943-971"},"PeriodicalIF":0.0,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00161g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990351","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
0
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
相关产品
×
本文献相关产品
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信
小红书