JACS Au最新文献

{"title":"Reversing the Rate versus Overpotential Scaling in Electrocatalytic Hydrogen Evolution Induced by Electrostatic Field Engineering at Remote Sites","authors":"Anannya Saha,&nbsp;Shikha Ravish,&nbsp;Simarjeet Kaur,&nbsp;Jyoti Devi,&nbsp;Sayantan Paria,&nbsp;Suman K. Barman","doi":"10.1021/jacsau.6c00424","DOIUrl":"https://doi.org/10.1021/jacsau.6c00424","url":null,"abstract":"<p>The rate versus overpotential relationship arising frommolecularscaling effects is a key challenge in developing efficient electrocatalysts.Circumventing these unyielding scaling relationships is a persistentchallenge in the field of electrocatalysis. Escaping this iron lawof rate versus overpotential requires judicious modulation, whichcan balance the electrophilic and nucleophilic/basic characteristicsof the electrocatalyst, which is rarely straightforward. Here, wereport <em>local electrostatic field-persuaded inverse scaling relationships</em> of the electrocatalytic hydrogen evolutionreaction (HER). For this purpose, we report six mononuclear Ni^II complexes <strong>1</strong>–<strong>6</strong>, where <strong>4</strong>, <strong>5</strong>, and <strong>6</strong> contain positively chargedquaternary ammonium moieties at remote sites. Without perturbing theprimary coordination sphere, this molecular scaffold allows the installationof a local positive charge, which would increase the electrophiliccharacter, favoring electron transfer processes. This is reflectedby the anodic shift in the reductive redox potentials from neutralto charge-appended complexes (<strong>1</strong> to <strong>6</strong>). Sincethe catalytically relevant anionic/reduced species are achieved easilyvia electrostatic stabilization by the local positive charge, thisleads to a lower overpotential. Density functional theory (DFT) calculationsreveal that the appended local positive charge facilitates the r.d.s.step by ground-state destabilization of the starting intermediate,which leads to a lower activation barrier and facilitates the HER.Thus, the present study demonstrates the optimum balance between theelectrophilic character and basicity of the electrocatalyst, assistedby the local positive charge, leading to inverse scaling relationships.To the best of our knowledge, this is the first demonstration of apositive electrostatic field-assisted enhanced HER activity with agradual decrease in overpotential.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"6 9","pages":"4929–4943"},"PeriodicalIF":8.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149071054","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synergistic Computational–Experimental Discovery of a Zwitterionic Fused-Ring High-Energy-Density Material with Intrinsic Insensitivity","authors":"Bojun Tan,&nbsp;Jing Zhang,&nbsp;Linhu Pan,&nbsp;Siwei Song,&nbsp;Changwei Tang,&nbsp;Binghui Duan,&nbsp;Xiong Yang,&nbsp;Min Gao,&nbsp;Shuai Wang,&nbsp;Chenqi Shi,&nbsp;Jinkang Dou,&nbsp;Qinghua Zhang,&nbsp;Ning Liu","doi":"10.1021/jacsau.6c00567","DOIUrl":"https://doi.org/10.1021/jacsau.6c00567","url":null,"abstract":"<p>The relentless pursuitof high-energy-density materials (HEDMs)is fundamentally constrained by the inherent trade-off between energyoutput and molecular stability. Nitrogen-rich fused-ring scaffoldshave emerged as a privileged platform to navigate this challenge,yet the systematic exploration of their chemical space and the rationaldesign of derivatives that simultaneously achieve high energy, lowsensitivity, and favorable physicochemical properties remain elusive.Herein, we report a synergistic computational–experimentalstrategy that integrates high-throughput screening with rational moleculardesign to discover a new class of [5,6,5] fused-ring energetic zwitterions.Starting from a combinatorially enumerated library of nearly ten million[5,6,5] fused-ring structures, we employed a validated performance-predictionmodel─incorporating machine learning and quantum chemical calculations─toiteratively screen for candidates with an optimal balance of highdensity, low impact sensitivity, and high thermal stability. Thisprocess identified a unique structural motif that merges the stabilizingconjugation of a planar, nitrogen-rich fused framework with the dense-packingadvantages of a zwitterionic architecture, effectively addressingthe long-standing acidity issue associated with traditional NTO-basedmaterials. This guided approach culminated in the successful synthesisof a lead compound, <strong>TYX-7.</strong> Critically, <strong>TYX-7</strong> exhibits a measured density of 1.95 g/cm³, a detonationvelocity of 9.113 km/s, a detonation pressure of 35.4 GPa─performancemetrics on par with HMX─along with low mechanical sensitivity(IS &gt; 40 J, FS &gt; 360 N) while retaining the low sensitivitycharacteristicof NTO. Beyond its impressive energetic performance, <strong>TYX-7</strong> demonstrates exceptionally low ignition delay (130.0 ms at 70 W/cm²), sustained and stable combustion over extended durations,and remarkably clean burning with minimal smoke generation, underscoringits promise for practical applications. Its measured p<em>K</em>_a of 5.99 signifies a remarkable shift toward neutrality,overcoming the corrosive drawback of its predecessor. This work notonly delivers a promising new HEDM candidate but also establishesa robust, transferable paradigm for the accelerated discovery anddesign of next-generation energetic materials.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"6 9","pages":"4980–4992"},"PeriodicalIF":8.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067453","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Hydrogen Spillover from Pt, Pd, and Au Evaluated with MnOx Temperature-Programmed Reduction","authors":"Mohammad Hamidizirasefi,&nbsp;Audrey M. Battiste,&nbsp;Angela Pathickal Abraham,&nbsp;Andersen P. Dimon,&nbsp;Bert D. Chandler","doi":"10.1021/jacsau.6c00822","DOIUrl":"https://doi.org/10.1021/jacsau.6c00822","url":null,"abstract":"<p>Hydrogen spillover occurs when H₂ adsorbson an activemetal and is then transferred to a reducible metal oxide. While spilloveris involved in many catalytic reactions, fundamental studies of spilloverhave been limited by the paucity of experimental methods availableto study it. Here, we develop an experimental temperature-programmedreduction (TPR) protocol to rapidly compare spillover from differentmetals (Pt, Pd, Au ) onto P25 titania, using MnO_<em>x</em> reduction probe reaction. X-ray photoelectron and UV–visiblespectroscopies indicated reduction to MnO in the presence and absenceof active metals, and quantitative H₂ consumption measurementswere consistent across all samples. Observed MnO_<em>x</em> reduction temperatures, which decrease by shifting as muchas 150 °C, depend strongly on the metal loading and confirm H₂ activation occurs at metal sites. Adding only 300 ppm Aucaused the Kissinger apparent activation energy to decrease from 55to &lt;10 kJ/mol. Comparisons across metals and loadings indicatethat MnO_<em>x</em> reduction is limited by H₂ activation only at very low metal loadings and temperatures.Gold induces the largest shift in MnO_<em>x</em> reduction, indicating that it is the most competent spillover metalunder these conditions. At moderately higher loadings (≥1 site/100nm²), Pt and Au become equivalent, signaling that MnO_<em>x</em> reduction is no longer limited by H₂ activation at higher metal loadings. Palladium is moderatelyslower, consistent with the generation of a PdH_<em>x</em> phase at low temperature. At higher active site loadings,MnO_<em>x</em> reduction depends primarily on thesurface concentration of spillover H, providing a simple and usefulapproach for comparing catalysts.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"6 9","pages":"5179–5189"},"PeriodicalIF":8.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067526","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electricity-Controlled Divergent Synthesis of CF3-Tethered Pyrazolines and Pyrazoles via Tandem Radical Trifluoromethylation and Annulation","authors":"Paramita Pattanayak,&nbsp;Yogesh K. Girase,&nbsp;Tanmay Chatterjee","doi":"10.1021/jacsau.6c00788","DOIUrl":"https://doi.org/10.1021/jacsau.6c00788","url":null,"abstract":"<p>Electricity-controlled, diversity-oriented selectivesynthesisis a powerful strategy for accessing structurally distinct potentialorganic molecules. However, achieving this transformation remainsa significant challenge in synthetic chemistry. Herein, we reporta metal- and external-oxidant-free electrochemical strategy that enablesthe highly selective synthesis of CF₃-tethered pyrazolinesand pyrazoles (&gt;45 examples) from readily available <em>N</em>-allyl-<em>N</em>’-benzylidenesulfonohydrazides andCF₃SO₂Na. This protocol operates via a tandemsequence involving regioselective radical trifluoromethylation, annulation,and oxidation. Notably, precise control over product selectivity isachieved simply by modulating the applied current under constant-currentelectrolysis conditions. As a result, <em>N</em>-sulfonylpyrazolines, <em>N</em>-sulfonyl pyrazoles, and <em>N</em>–H pyrazoles are selectively synthesized from the same startingmaterials. The method features broad substrate scope and functional-grouptolerance, including derivatives of fragrances, pharmaceuticals, andnatural products. Electricity serves as the sole reagent, with H₂ as a benign byproduct, demonstrating the protocol’shigh sustainability. Mechanistic investigations support a radical-mediatedpathway involving a ^•CF₃-radical. Interestingly,electron-rich heteroaryl-substituted sulfonohydrazides preferentiallyundergo C–H trifluoromethylation of the heteroaryl moiety ratherthan annulation. This observation highlights the differential reactivityof the ^•CF₃ radical toward (hetero)aryl-substituted <em>N</em>-allylsulfonohydrazides.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"6 9","pages":"5118–5129"},"PeriodicalIF":8.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067505","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Photoinduced Accumulative Electron-Transfer Dynamics in Perylene Diimide Polymers as Photoredox Catalysts","authors":"Zicong Situ,&nbsp;Xingqing Li,&nbsp;Ying-Xin Qiao,&nbsp;Chao Yang,&nbsp;Yanqi Chen,&nbsp;Mengke Tang,&nbsp;Yang Li,&nbsp;Yan Wan,&nbsp;Hongwei Song,&nbsp;Qing-Xiao Tong,&nbsp;Jing-Xin Jian,&nbsp;Zhuoran Kuang","doi":"10.1021/jacsau.6c00868","DOIUrl":"https://doi.org/10.1021/jacsau.6c00868","url":null,"abstract":"<p>Understanding the mechanisms of light-driven charge separation(CS), accumulative electron transfer, and free carrier (FC) dynamicsin polymer semiconductors as photoredox catalysts is essential forartificial photosynthesis and for developing efficient solar energyconversion materials. This study presents a comparative investigationon the photoinduced electron transfer dynamics of three perylene diimide(PDI) polymers, <em><strong>o</strong></em> <strong>PDI</strong>, <em><strong>m</strong></em> <strong>PDI</strong>, and <em><strong>p</strong></em> <strong>PDI</strong>, that differ by their phenylenediaminelinkers. Notably, <em><strong>o</strong></em> <strong>PDI</strong>,which is constructed with <em>ortho</em>-phenylenediaminelinkers, exhibits the fastest two-electron CS and the subsequent FCgeneration among this series. These superior properties are attributedto its large molecular dipole moment and driving force for multielectronaccumulation. The high photocatalytic activity of <em><strong>o</strong></em> <strong>PDI</strong> was further verified through two independenttwo-electron quenching experiments and the oxygen reduction reaction(ORR). The latter efficiently generates H₂O₂, particularly in the case of <em><strong>o</strong></em> <strong>PDI</strong>, leading to the rapid degradation of uric acid (UA). Thiswork elucidates the mechanism of photoinduced accumulative electrontransfer in PDI-based polymers and provides a theoretical frameworkfor the rational design of efficient multielectron accumulation systemsin advanced photocatalytic applications.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"6 9","pages":"5214–5224"},"PeriodicalIF":8.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067551","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Divergent Iron Catalysis with Zincke Imines: Access to C5-Amidated Pyridines and Oxazole Derivatives from 2-Substituted Pyridines","authors":"Abuthayir Mohamathu Ghouse,&nbsp;Sidda Manoj,&nbsp;Shafiya,&nbsp;Cherumannil Femina,&nbsp;Sridhar Balasubramanian,&nbsp;Resmi K. R.,&nbsp;Pookkottu K. Sajith,&nbsp;Srirama Murthy Akondi","doi":"10.1021/jacsau.6c00765","DOIUrl":"https://doi.org/10.1021/jacsau.6c00765","url":null,"abstract":"<p>The transformationof electron-deficient pyridines intoelectron-richZincke imines is a well-established strategy for selective C3/C5 functionalizationvia electrophilic or radical pathways. Despite this, the reactivityof these imines toward metal nitrenoids has remained unexplored. Addressingthis gap, we herein disclose an iron-catalyzed divergent reactionof Zincke imines with dioxazolones. Depending on the conditions, thisprotocol provides access to either C5-amidopyridines or substitutedoxazoles, primarily starting from 2-substituted pyridines. This highlyregioselective C5-amidation proceeds under mild conditions to furnishbiologically relevant 2-substituted 5-amidopyridines, providing directaccess to valuable scaffolds that are otherwise challenging and costlyto access via conventional routes. Conversely, oxidative conditionsat elevated temperatures favor the formation of oxazole derivativeswith versatile synthetic handles. Mechanistic and theoretical insightssupport the generation of a reactive Fe(III)-imidyl intermediate thatundergoes selective addition at the C5 position of the Zincke imine.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"6 9","pages":"5081–5092"},"PeriodicalIF":8.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067553","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Solid-State Dynamic Behavior of the Boron–Nitrogen Bond Enables Mechanophotocatalysis of a [2 + 2]-Photocycloaddition","authors":"Alaric Shaw,&nbsp;Peter F. Gilbert,&nbsp;Ivan Bondarenko,&nbsp;Kokoro K. Holcomb,&nbsp;Paulina M. Sittinger,&nbsp;Jesus Daniel Loya,&nbsp;Simon J. Teat,&nbsp;Nicholas S. Settineri,&nbsp;Gonzalo Campillo-Alvarado","doi":"10.1021/jacsau.6c00942","DOIUrl":"https://doi.org/10.1021/jacsau.6c00942","url":null,"abstract":"<p>We report reversibleB←N coordinate bond formationand cleavagein the organic solid state. The dynamic behavior was probed usingthe [2 + 2]-photodimerization of 4-(1-naphthylvinyl)pyridine (<strong>4-nvp</strong>) as a chemical reporter under concurrent mechanochemicalvortex grinding and ultraviolet light-emitting diode (UV-LED) irradiation.Phenylboronic acid catechol ester (<strong>pbe</strong>) templates theregio- and stereoselective formation of 1,3-bis(4-pyridyl)-2,4-bis(1-naphthyl)cyclobutane(<strong>pncb</strong>), and the reaction proceeds efficiently even when <strong>pbe</strong> is used in substoichiometric amounts (50%, 30% and 5%mol). The catalytic turnover demonstrates that B←N bonds canbreak and reform dynamically under mechanical stress in the organicsolid state, establishing B←N coordination as a design elementfor responsive molecular materials.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"6 9","pages":"4897–4902"},"PeriodicalIF":8.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067555","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"MacroTox: A Macroscopic Graph Topology-Based Multimodal Learning Framework for Robust Molecular Toxicity Prediction","authors":"He Huang,&nbsp;Qinyi Wang,&nbsp;Manzhan Zhang,&nbsp;Pan Dou,&nbsp;Xiaobo Yang,&nbsp;Honglin Li,&nbsp;Shiliang Li","doi":"10.1021/jacsau.6c01105","DOIUrl":"https://doi.org/10.1021/jacsau.6c01105","url":null,"abstract":"<p>Despite breakthroughs in predicting acute organ toxicities,advancedcomputational models continue to struggle with complex, insidiousend points like drug-induced bone toxicity. A fundamental limitationof most supervised pipelines is their failure to explicitly modelintermolecular similarities during task-specific training. Neglectingthis macroscopic topology of the chemical space leads to fragmentedlatent representations, poor generalization, and high false negativerates. To address this, we propose MacroTox, a macroscopic topology-drivenmultimodal deep learning framework. Beyond intramolecular fusion,its core innovation is the dynamic construction of an intrabatch drug–drugsimilarity graph. Guided by a topology-aware synergistic optimization,this mechanism captures latent network correlations, maximizing theutilization of the chemical space to resolve representational fragmentationand enhance the predictive capacity under data scarcity. Evaluatedona rigorously curated bone toxicity data set, MacroTox achieved anarea under the receiver operating characteristic curve of 0.93 anda Matthews correlation coefficient of 0.73. Crucially, it effectivelybalances the sensitivity-specificity trade-off (SEN: 0.88, SPE: 0.86),substantially mitigating the underreporting risks in bone toxicityscreening. Notably, ablation studies confirm that these predictiveenhancements stem from the synergistic effect of dynamic graph topologyand edge loss regularization. Extensive benchmarking of MoleculeNetfurther confirms its robust transferability. Furthermore, via multilevelfeature attribution, MacroTox elucidates chemically intuitive structure–activityrelationships. By pinpointing specific toxicophores and resolvingcomplex activity cliffs, the framework proves that it captures authentictoxicological mechanisms rather than memorizing superficial data setbiases. Ultimately, MacroTox offers an reliable, generalizable, andinterpretable virtual screening engine for early stage drug discovery.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"6 9","pages":"5420–5432"},"PeriodicalIF":8.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067527","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Competition-Derived Relative Reactivity and 3D Electronic-State Analysis of Site- and Facial Selectivity in NaBH4/MeOH Ketone Reductions","authors":"Daimon Sakaguchi,&nbsp;Taisei Kawasaki,&nbsp;Mayu Itakura,&nbsp;Chihiro Tada,&nbsp;Hiroaki Gotoh","doi":"10.1021/jacsau.6c01269","DOIUrl":"https://doi.org/10.1021/jacsau.6c01269","url":null,"abstract":"<p>Yield-based measuresof reactivity can be distorted by side reactionsand reaction conditions and therefore may not accurately reflect intrinsicreaction rates. In this study, competition experiments, in which twosubstrates react simultaneously with the same reagent, were used tobuild a unified kinetic scale for the reduction of ketones by sodiumborohydride (NaBH₄) in methanol, expressed as activationfree energy differences (ΔΔ<em>G</em>^‡). Kinetic data for 89 structurally diverse ketone reaction facestracked substituent electronic effects and steric congestion, andtransition-state calculations identified methanolysis as the stepthat determines the identity of the active reductant. A Lasso modeltrained on 83 of these reaction faces with three-dimensional electron-density,electrostatic-potential, and carbonyl-centered projected C═Oπ* descriptors achieved <em>R</em>² = 0.804under strict nested outer leave-one-out cross-validation. The monoketone-derivedmodel recovers the dominant site and face for every diketone examined,with 85.5% of the cross-validation models reproducing all assignments;however, the predicted product distributions are indicative ratherthan quantitative. The workflow integrates a yield-independent kineticscale with experimental measurements, theoretical calculations, anddata-driven analyses within the evaluated NaBH₄/MeOH domainand provides a basis for testing broader applicability through reaction-specificdata, retraining, and validation.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"6 9","pages":"5465–5477"},"PeriodicalIF":8.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067499","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Bridging the Gap Between Laboratory Catalyst Research and Practical Water Electrolyzer Commercialization","authors":"Sujin Park,&nbsp;Tianshu Gao,&nbsp;Hyeseong Jeon,&nbsp;Nanfeng Zheng,&nbsp;Hyunjoo Lee,&nbsp;Hua Bing Tao","doi":"10.1021/jacsau.6c01104","DOIUrl":"https://doi.org/10.1021/jacsau.6c01104","url":null,"abstract":"<p>Water electrolyzersare key technologies for enabling a carbon-neutralsociety by facilitating sustainable hydrogen production. Despite extensiveefforts to develop highly active catalysts, a persistent gap remainsbetween catalyst performance evaluated in rotating disk electrode(RDE) systems and that achieved in practical membrane electrode assembly(MEA) configurations. In this perspective, we highlight the originsof this discrepancy and emphasize that intrinsic catalytic activityalone is insufficient to predict electrolyzer performance. Using theacidic hydrogen evolution reaction (HER) as a model system, we demonstratethat apparent activity metrics such as mass activity and Tafel slopecan be significantly influenced by catalyst loading, composition,and measurement conditions in RDE, often leading to misleading conclusions.In contrast, MEA performance is governed by complex interfacial phenomenaincluding mass, electron, and charge transport. A similar behaviorwas also observed for alkaline HER and acidic oxygen evolution reaction(OER). We further present case studies illustrating the critical rolesof electron transfer and durability in water electrolyzers. In addition,recent advances in proton-exchange-membrane water electrolyzer commercializationare discussed, highlighting the importance of system-level optimization,including ionomer distribution control and scalable manufacturingvia slot-die coating, which enabled the deployment of a 2.5 MW system.Overall, bridging the gap between laboratory catalyst research andindustrial water electrolyzer applications requires a shift from catalyst-centricdesign toward integrated system-level engineering.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"6 9","pages":"4875–4887"},"PeriodicalIF":8.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067544","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}