EES catalysisPub Date : 2025-01-02DOI: 10.1039/D4EY00258J
Xueli Yan, Li Tian, Fei Xue, Jie Huang, Rui Zhao, Xiangjiu Guan, Jinwen Shi, Wenshuai Chen and Maochang Liu
{"title":"In situ hydrogen production in all-level-humidity air: integrating atmospheric water harvesting with photocatalysis†","authors":"Xueli Yan, Li Tian, Fei Xue, Jie Huang, Rui Zhao, Xiangjiu Guan, Jinwen Shi, Wenshuai Chen and Maochang Liu","doi":"10.1039/D4EY00258J","DOIUrl":"https://doi.org/10.1039/D4EY00258J","url":null,"abstract":"<p >H<small><sub>2</sub></small> production from air holds great promise as a sustainable method for green energy harvesting. However, its widespread adoption faces challenges in realizing mobile, distributed, community-managed, off-grid <em>in situ</em> H<small><sub>2</sub></small> production systems. Here, we report a bilayer nanofibrillated cellulose composite gel incorporating lithium chloride hygroscopic salt and a supported SrTiO<small><sub>3</sub></small>:Al photocatalyst (denoted as NLS), designed specifically for <em>in situ</em> photocatalytic splitting of atmospheric water to produce H<small><sub>2</sub></small>, using only naturally occurring moisture and sunlight. The NLS gel features a self-supply of atmospheric water, spectral splitting for efficient solar energy delivery and complementary utilization, instantaneous H<small><sub>2</sub></small> evolution, and stable catalyst immobilization. As a result, the NLS bilayer gel successfully achieves <em>in situ</em> H<small><sub>2</sub></small> production in full-range-humidity environments, demonstrating a hygroscopicity of 4.26 g<small><sub>H<small><sub>2</sub></small>O</sub></small> g<small><sub>sorbent</sub></small><small><sup>−1</sup></small> and an H<small><sub>2</sub></small> production activity of 65.45 μmol h<small><sup>−1</sup></small> in a 90% relative humidity environment, achieving a solar-to-hydrogen efficiency of up to 0.3%. This work represents a promising step towards realizing <em>in situ</em> H<small><sub>2</sub></small> production from air across varying humidity levels, independent of geographical constraints.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 2","pages":" 297-304"},"PeriodicalIF":0.0,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00258j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143564281","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}
EES catalysisPub Date : 2024-12-27DOI: 10.1039/D4EY00190G
Jan-Willem Hurkmans, Henri M. Pelzer, Tom Burdyny, Jurriaan Peeters and David A. Vermaas
{"title":"Heating dictates the scalability of CO2 electrolyzer types†","authors":"Jan-Willem Hurkmans, Henri M. Pelzer, Tom Burdyny, Jurriaan Peeters and David A. Vermaas","doi":"10.1039/D4EY00190G","DOIUrl":"10.1039/D4EY00190G","url":null,"abstract":"<p >Electrochemical CO<small><sub>2</sub></small> reduction offers a promising method of converting renewable electrical energy into valuable hydrocarbon compounds vital to hard-to-abate sectors. Significant progress has been made on the lab scale, but scale-up demonstrations remain limited. Because of the low energy efficiency of CO<small><sub>2</sub></small> reduction, we suspect that significant thermal gradients may develop in industrially relevant dimensions. We describe here a model prediction for non-isothermal behavior beyond the typical 1D models to illustrate the severity of heating at larger scales. We develop a 2D model for two membrane electrode assembly (MEA) CO<small><sub>2</sub></small> electrolyzers; a liquid anolyte fed MEA (exchange MEA) and a fully gas fed configuration (full MEA). Our results indicate that full MEA configurations exhibit very poor electrochemical performance at moderately larger scales due to non-isothermal effects. Heating results in severe membrane dehydration, which induces large Ohmic losses in the membrane, resulting in a sharp decline in the current density along the flow direction. In contrast, the anolyte employed in the exchange MEA configuration is effective in preventing large thermal gradients. Membrane dehydration is not a problem for the exchange MEA configuration, leading to a nearly constant current density over the entire length of the modeled domain, and indicating that exchange MEA configurations are well suited for scale-up. Our results additionally indicate that a balance between faster kinetics, higher ionic conductivity, smaller pH gradients and lower CO<small><sub>2</sub></small> solubility causes an optimum operating temperature between 60 and 70 °C.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 2","pages":" 305-317"},"PeriodicalIF":0.0,"publicationDate":"2024-12-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11721209/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142973594","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}
{"title":"Quantifying the prospect of a visible-light-absorbing oxysulfide photocatalyst by probing transient absorption and photoluminescence†","authors":"Ryota Shoji, Vikas Nandal, Kazuhiko Seki, Xiaoping Tao, Akihiro Furube, Takashi Hisatomi, Hiroaki Yoshida, Tsuyoshi Takata, Masanori Kaneko, Koichi Yamashita, Kazunari Domen and Hiroyuki Matsuzaki","doi":"10.1039/D4EY00187G","DOIUrl":"https://doi.org/10.1039/D4EY00187G","url":null,"abstract":"<p >Photocatalytic water splitting is an emerging renewable technology for producing green hydrogen fuel from sunlight and water on a large scale. Identifying charge-carrier transport properties is critical for establishing a design pathway for exciting visible-light-absorbing oxysulfide-based photocatalysts. Herein, the dynamics of distinct charge carriers in the Gd<small><sub>2</sub></small>Ti<small><sub>2</sub></small>O<small><sub>5</sub></small>S<small><sub>2</sub></small> (GTOS) photocatalyst is revealed by transient optical spectroscopies (transient diffuse reflectance (TDR) and transient photoluminescence (TPL) spectroscopies) and theoretical modeling. We demonstrate that TDR and TPL signals can probe the evolution of photoexcited mobile electrons and holes separately for GTOS. The decay of optical signals primarily originates from bimolecular recombination of mobile electrons with detrapped holes from shallow trap states close to the valence band. Using different estimated parameters, the effects of the size reduction and charge carrier extraction rate <em>k</em><small><sub>e</sub></small> (surface to electrolyte) on the internal quantum efficiency (IQE) are determined. Our results indicate that the IQE can be tremendously improved by simultaneously reducing particle size and increasing <em>k</em><small><sub>e</sub></small>. After particle size reduction, we show that the high apparent quantum yield (∼30%) GTOS was achieved by improving <em>k</em><small><sub>e</sub></small> (from surface treatment and optimizing the cocatalyst loading method) as compared to Y<small><sub>2</sub></small>Ti<small><sub>2</sub></small>O<small><sub>5</sub></small>S<small><sub>2</sub></small> (0.7%). Our work presents a comprehensive methodology that identifies the critical photophysical properties of visible-light-absorbing photocatalysts for efficient and scalable particulate photocatalyst-based solar water splitting systems.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 2","pages":" 274-285"},"PeriodicalIF":0.0,"publicationDate":"2024-12-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00187g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143564275","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}
{"title":"Integrating oxophilic and protophilic properties in a multivalent Co9S8@CoMoPx electrode to boost alkaline hydrogen evolution†","authors":"Xijie Chen, Fengming Zhang, Xiao Wang, Fangming Liu, Jinhan Li, Meng Yu and Fangyi Cheng","doi":"10.1039/D4EY00252K","DOIUrl":"https://doi.org/10.1039/D4EY00252K","url":null,"abstract":"<p >The alkaline hydrogen evolution reaction (HER) is plagued by intricate interfacial reactions involving the dissociation of interfacial H<small><sub>2</sub></small>O molecules and adsorption/desorption of H<small><sub>ads</sub></small>/OH<small><sub>ads</sub></small> species, which impede the practical application of water electrolysis. Herein, a self-supported Co<small><sub>9</sub></small>S<small><sub>8</sub></small>@CoMoP<small><sub><em>x</em></sub></small> electrode with a nanosheet cluster morphology was developed using a stepwise electrodeposition method for an efficient electrocatalytic HER. Benefiting from the coexistence of multivalent metal sites, the Co<small><sub>9</sub></small>S<small><sub>8</sub></small>@CoMoP<small><sub><em>x</em></sub></small> electrode integrated both oxophilic and protophilic properties to facilitate the cracking of molecular H<small><sub>2</sub></small>O and subsequent hydrogen generation. As a result, the obtained Co<small><sub>9</sub></small>S<small><sub>8</sub></small>@CoMoP<small><sub><em>x</em></sub></small> electrode exhibited superior alkaline HER activities, delivering an overpotential of 226 mV at −500 mA cm<small><sup>−2</sup></small> with a low attenuation rate of 11 μV h<small><sup>−1</sup></small> after 1000 h. An anion-exchange membrane water electrolysis device was then assembled by matching the Co<small><sub>9</sub></small>S<small><sub>8</sub></small>@CoMoP<small><sub><em>x</em></sub></small> cathode with an NiFe-based anode to demonstrate its industrial application potential. This work emphasizes the significance of constructing multivalent metal sites to simultaneously achieve oxophilicity and protophilicity, providing a guideline for the rational design of heterostructure electrocatalysts for efficient energy conversion.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 2","pages":" 259-267"},"PeriodicalIF":0.0,"publicationDate":"2024-12-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00252k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143564273","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}
EES catalysisPub Date : 2024-12-18DOI: 10.1039/D4EY90027H
Shi-Zhang Qiao
{"title":"EES Catalysis: embracing energy and environmental catalysis","authors":"Shi-Zhang Qiao","doi":"10.1039/D4EY90027H","DOIUrl":"https://doi.org/10.1039/D4EY90027H","url":null,"abstract":"<p >Welcome to the first issue of <em>EES Catalysis</em> in 2025! As we enter this new year, we reflect on the remarkable journey since our launch in 2023. With a strong year in 2024, <em>EES Catalysis</em> has grown into a dynamic platform for groundbreaking research and a thriving community dedicated to advancing energy and environmental catalysis. In this Editorial, we are excited to highlight recent achievements and share our vision for the promising future of <em>EES Catalysis</em>.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 8-9"},"PeriodicalIF":0.0,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey90027h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142994074","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}
{"title":"Selective electroreduction of CO2 to formate by a heterogenized Ir complex using H2O as an electron/hydrogen source†","authors":"Jieun Jung, Keun Woo Lee, Naonari Sakamoto, Selvam Kaliyamoorthy, Taku Wakabayashi, Kenji Kamada, Keita Sekizawa, Shunsuke Sato, Tomiko M. Suzuki, Takeshi Morikawa and Susumu Saito","doi":"10.1039/D4EY00261J","DOIUrl":"https://doi.org/10.1039/D4EY00261J","url":null,"abstract":"<p >A newly synthesized tetradentate PNNP-coordinated iridium (Ir) complex, Mes-IrPPh2, immobilized on a carbon material, was found to be a superior catalyst for CO<small><sub>2</sub></small> electrochemical reduction reaction (CO<small><sub>2</sub></small>ERR) to give formate, (HCOO<small><sup>−</sup></small>), allowing an operation near the theoretical potential (−0.18 V <em>vs.</em> RHE, pH = 7.3) in water. The combined [Mes-IrPPh2] electrode furnished HCOO<small><sup>−</sup></small> with a current density of greater than 2.2 to 7.7 mA cm<small><sup>−2</sup></small> over −0.27 to −0.47 V <em>vs.</em> RHE, providing faradaic efficiencies (FE) of >90%. The outstanding robustness of the electrode attained continuous production of HCOO<small><sup>−</sup></small> up to 12.5 mmol with 2.86 μmol of Mes-IrPPh2 at −0.27 V <em>vs.</em> RHE over 168 h. Furthermore, solar-driven electrochemical CO<small><sub>2</sub></small> reduction to HCOO<small><sup>−</sup></small> was also carried out in water with a Ni/Fe–Ni foam anode as a water oxidation catalyst and a silicon photovoltaic cell to achieve a solar-to-formate conversion efficiency (<em>η</em><small><sub>STF</sub></small>) of 13.7%.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 2","pages":" 254-258"},"PeriodicalIF":0.0,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00261j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143564272","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}
EES catalysisPub Date : 2024-12-03DOI: 10.1039/D4EY00145A
Ping Niu, Haoqing Zhang, Jian Zeng, Tianjian Hu, Meixue Zhang, Chengyao Xie, Boyin Zhai, Jérémy Odent, Shulan Wang and Li Li
{"title":"Carbon incorporated isotype heterojunction of poly(heptazine imide) for efficient visible light photocatalytic hydrogen evolution†","authors":"Ping Niu, Haoqing Zhang, Jian Zeng, Tianjian Hu, Meixue Zhang, Chengyao Xie, Boyin Zhai, Jérémy Odent, Shulan Wang and Li Li","doi":"10.1039/D4EY00145A","DOIUrl":"https://doi.org/10.1039/D4EY00145A","url":null,"abstract":"<p >Clean hydrogen production using renewable solar energy is an important aspect in the development of a sustainable society. The premise of developing highly efficient photocatalysts for hydrogen production relies on achieving smooth charge carrier kinetics with efficient visible light absorption. Constructing isotype heterojunctions with structural or compositional similarity can enhance charge carrier separation at the interface, leading to improved utilization of light energy. However, this approach is often constrained by the availability as well as intrinsic properties of monomers. Herein, carbon facilitated <em>in situ</em> fabrication of an isotype heterojunction based on a poly(heptazine imide) (PHI) structure with high crystallinity and extended π-conjugation was proposed by calcinating carbon-modified melon in the “semi-liquid” NaCl/KCl salt. The heterojunction effect induced by the visible light responsive Na–PHI and K–PHI, as well as the strong charge coupling between heptazine and carbon ring in the covalent interface forms multi-directional built-in electric field and effectively promotes the separation of charge carriers. Together with the visible light absorption extension by simultaneous carbon ring decoration, C@Na–PHI/K–PHI shows superior photocatalytic hydrogen evolution activities under visible light irradiation and the apparent quantum efficiencies reach 29.3% and 3% under 420 and 550 nm, respectively. This study pioneers the idea and provides a useful reference for the design of PHI isotype heterojunctions for the effective utilization of solar energy.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 119-127"},"PeriodicalIF":0.0,"publicationDate":"2024-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00145a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142994107","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}
{"title":"Unidirectional bubble transportation on slippery micro-cone array electrodes enables spontaneous 99.99% gas separation in membrane-less water electrolysis†","authors":"Linfeng Yu, Yingze Yang, Pengpeng Xie, Qingzhen Xu, Anuj Kumar, Liang Luo, Hui Li, Haijun Xu, Haohong Duan and Xiaoming Sun","doi":"10.1039/D4EY00184B","DOIUrl":"https://doi.org/10.1039/D4EY00184B","url":null,"abstract":"<p >Membrane-less electrolysis is utilized for many gaseous chemical productions. However, the problems of gas mixing and low energy efficiency remain huge obstacles for its practical application. Herein, we have prepared a biomimetic electrode by three-dimensional (3D) printing technology, featuring a “slippery aerophobic” surface and micro-cone array structure with tunable tilting angles. These electrodes enable the bubbles that are generated at the cone tip to “roll-up” rapidly along the electrode towards its base, rather than being directly released into the electrolyte, resulting in gas mixing. The unidirectional bubble transportation behavior was understood by a collective analysis of the Laplace pressure on cones, bubble buoyancy and irreversible hysteresis. As a proof of concept, we employed this biomimetic electrode in membrane-less water electrolysis. At a current density of 240 mA cm<small><sup>−2</sup></small>, we achieved the separation of H<small><sub>2</sub></small> and O<small><sub>2</sub></small> gases with >99.99% purity even with an electrode distance as short as 1.5 mm. This work demonstrated the efficiency of precisely manipulating bubble transportation in membrane-less electrolysis that does not rely on expensive membranes.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 152-160"},"PeriodicalIF":0.0,"publicationDate":"2024-11-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00184b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142994110","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}
EES catalysisPub Date : 2024-11-22DOI: 10.1039/D4EY00204K
Jia Liu, Xiaoge Peng, Xiaosa Wang, Xing Zhong and Jianguo Wang
{"title":"Electrochemical ozone production: from fundamental mechanisms to advanced applications","authors":"Jia Liu, Xiaoge Peng, Xiaosa Wang, Xing Zhong and Jianguo Wang","doi":"10.1039/D4EY00204K","DOIUrl":"https://doi.org/10.1039/D4EY00204K","url":null,"abstract":"<p >Electrochemical ozone production (EOP) as an advanced ozone generation technology with good safety, simple equipment and high ozone concentration has sparked considerable interest among researchers. However, the unfavorable thermodynamics and sluggish kinetics have restricted EOP from widespread application. Developing low-cost and robust catalysts is crucial to solving the efficiency problem during the EOP process. Besides the catalyst aspect, the development of an advanced electrolyzer can further promote the large-scale utilization of the EOP process. However, there have been few systematic reviews that comprehensively elucidated the progress made in advancing the EOP process to date. In this review, we firstly summarize the recent progress in understanding the EOP mechanism. The latest advances and effective strategies for designing efficient catalysts are then introduced. Moreover, the standards to evaluate the activity and stability for different EOP catalysts are provided. The influence of EOP electrolyzer design and operating conditions on the overall operation, as well as the progress and prospects in large-scale EOP applications are also demonstrated. This review aims to comprehensively explore the EOP process, providing both theoretical and experimental insights, and this will help to facilitate the advancement of efficient EOP large-scale application.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 2","pages":" 170-204"},"PeriodicalIF":0.0,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00204k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143564269","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}
EES catalysisPub Date : 2024-11-20DOI: 10.1039/D4EY00172A
Lujin Pan, Jiasheng Lu, Olivia Dunseath, Michal Ronovský, An Guo, Malte Klingenhof, Xingli Wang, Elisabeth Hornberger, Alex Martinez Bonastre, Harriet Burdett, Jonathan Sharman, Fabio Dionigi and Peter Strasser
{"title":"Unveiling the origins of the activity gap between rotating disk electrodes and membrane electrode assemblies: Pt seed-mediated iridium-doped octahedral platinum nickel catalysts for proton exchange membrane fuel cells†","authors":"Lujin Pan, Jiasheng Lu, Olivia Dunseath, Michal Ronovský, An Guo, Malte Klingenhof, Xingli Wang, Elisabeth Hornberger, Alex Martinez Bonastre, Harriet Burdett, Jonathan Sharman, Fabio Dionigi and Peter Strasser","doi":"10.1039/D4EY00172A","DOIUrl":"https://doi.org/10.1039/D4EY00172A","url":null,"abstract":"<p >Proton exchange membrane fuel cells (PEMFCs) offer energy solutions of high efficiency and low environmental impact. However, the sluggish kinetics of the oxygen reduction reaction (ORR) at the cathode limit their commercialization. Pt-based electrocatalysts, particularly octahedral (oh)PtNi bimetallic catalysts doped with additional transition metals, stand out as promising candidates for enhancing ORR rates and overall cell performance. A key challenge in the development and validation of active oh PtNi electrocatalysts is the unsuccessful translation of laboratory-scale catalyst test results, typically assessed using the rotating disk electrode (RDE) method, to practical applications in membrane electrode assembly (MEA) for PEMFCs. Here, we consider a new family of Ir-doped octahedral ORR fuel cell catalysts with very high RDE-based Pt mass activities. First, we designed the catalysts and tuned the catalyst layer properties to achieve the new state-of-the-art performance for oh-PtNi catalysts in PEMFCs. Still, a significant decrease in relative performance with respect to Pt/C when transitioning from RDE into an MEA-based cathode environment was observed. Thus, to better understand this performance loss, we investigated the effects of ionomer–catalyst interactions by adjusting the I/C ratio, the effect of temperature by applying RDE under high temperature, and the effects of acidity and high current density by applying and introducing the floating electrode technique (FET) to shaped nanoalloys. A severe detrimental effect was observed for high I/C ratios, with a behaviour contrasting reference commercial catalysts, while the negative effect of high temperatures was enhanced at low I/C. Based on this analysis, our study not only demonstrates a catalyst with enhanced ORR activity and specifically higher electrochemical surface area (ECSA) among oh-PtNi catalysts, but also provides valuable insights into overcoming MEA implementation challenges for these advanced fuel cell catalysts.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 128-139"},"PeriodicalIF":0.0,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00172a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142994108","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}