ACS Applied Energy Materials最新文献

{"title":"Non-Destructive Interfacial Engineering Using PDA–PPY-Coated SWCNTs and Tannic Acid for Synergistically Stabilized Silicon Anodes","authors":"Minwoo Choi,&nbsp;Juhyeong Cho,&nbsp;Neetu Bansal,&nbsp;Rahul R. Salunkhe,&nbsp;Heejoon Ahn","doi":"10.1021/acsaem.6c02099","DOIUrl":"https://doi.org/10.1021/acsaem.6c02099","url":null,"abstract":"<p>Silicon is a promising high-capacity anode material for next-generation lithium-ion batteries, but its severe volume expansion and low intrinsic conductivity induce interfacial instability, crack formation, and conductive-network failure. Herein, we present a non-destructive interfacial engineering strategy using single-walled carbon nanotubes (SWCNTs) conformally coated with a polydopamine–polypyrrole (PDA–PPY) copolymer and integrated into a tannic acid (TA)-reinforced carboxymethyl cellulose (CMC) binder matrix. The PDA–PPY coating improves SWCNT dispersion, hydrophilicity, and interfacial adhesion while preserving the integrity of the graphitic sp² framework. TA further establishes a multidentate hydrogen-bonding network among PDA–PPY, Si, and the CMC backbone, reinforcing conductive-network cohesion and suppressing structural degradation during repeated cycling. The coating chemistry and hydrogen-bonding network collectively regulate interfacial wettability, conductive-network morphology, and SEI evolution. As a result, the optimized Si@CMCTA PDA–PPY SW electrode retains 71.09% of its capacity after 100 cycles at 1 A g^–1 and 61.06% after 200 cycles at 2 A g^–1. Notably, it delivers 1148.95 mA h g^–1 even at 8 A g^–1, approximately 1.65 times that of the conventional CMC–SWCNT counterpart. Post-cycling XPS depth-profiling analysis further demonstrates suppressed crack formation and the formation of a thin, compact, LiF-rich interphase, indicating effective stabilization of the electrode/electrolyte interface.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 18","pages":"12483–12498"},"PeriodicalIF":5.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067575","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Heptazine-Based Polyimide with Dense Redox Sites and Large Conjugated Structure for Cathodic Lithium-Ion Storage","authors":"Peidong Liu,&nbsp;Jinghua Tan,&nbsp;Jie Huang,&nbsp;Pan He,&nbsp;Jieping Guo,&nbsp;Rong Du,&nbsp;Shaohua Xu,&nbsp;Qingpeng Zhao,&nbsp;Yiwu Liu","doi":"10.1021/acsaem.6c01411","DOIUrl":"https://doi.org/10.1021/acsaem.6c01411","url":null,"abstract":"<p>As organic cathode materials for lithium-ion batteries (LIBs), polyimides (PIs) have attracted widespread attention due to their abundant redox-active carbonyl sites, structural tunability, and environmental compatibility. However, the presence of electrochemically inactive structural units in conventional PIs limits their specific capacity. Herein, a novel heptazine-based polyimide (MePI) cathode for LIBs is prepared, which features dense redox sites and large conjugated structure, and its composites with multi-walled carbon nanotubes (MWCNTs) are prepared through an in situ solid-state thermal polymerization method. The composites exhibit improved electrochemical performance due to the enhanced conductivity and more accessible active sites provided by the carbon nanotubes. Among the prepared composites, MePI@MWCNT-50% achieves the highest specific capacity of 181 mAh g^–1 at 0.1 A g^–1 and maintains great cycling stability after 1000 cycles at 0.5 A g^–1. Ex situ FT-IR and density functional theory calculations reveal that heptazine rings serve as reversible Li⁺ storage sites. This work provides a promising strategy for the development of advanced organic electrodes for next-generation LIBs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 18","pages":"12225–12233"},"PeriodicalIF":5.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149071161","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Insight into Zn2+ Storage in Ti3C2Tx MXene within the Underpotential Deposition Region","authors":"Eugenio Gibertini,&nbsp;Prisca Viviani,&nbsp;Isheta Majumdar,&nbsp;Rossella Yivlialin,&nbsp;Gianlorenzo Bussetti,&nbsp;Andrea Lucotti,&nbsp;Luca Magagnin","doi":"10.1021/acsaem.6c01642","DOIUrl":"https://doi.org/10.1021/acsaem.6c01642","url":null,"abstract":"<p>The search for alternatives to Li-ion batteries is accelerating the development of aqueous Zn-based electrochemical energy-storage systems such as Zn-ion batteries and Zn-ion hybrid supercapacitors. Despite the increasing use of Ti₃C₂T_<em>x</em> MXene as an interfacial material for Zn electrochemistry, the mechanisms governing Zn²⁺ behavior in the underpotential deposition (UPD) regime remain poorly understood. Here, we present a comprehensive multitechnique investigation of Zn²⁺ storage on inkjet-printed Ti₃C₂T_<em>x</em> MXene thin films. Electrochemical analyses combined with low-scan-rate kinetic studies, in situ Raman spectroscopy, SEM, XRD, and XPS reveal the emergence of a surface-confined process between –0.8 and –1.0 V vs Ag/AgCl that precedes bulk Zn deposition. The collected evidence indicates Zn²⁺ adsorption coupled with partial charge transfer and the formation of a quasi-two-dimensional Zn adlayer or nanocluster phase stabilized by Ti=O surface terminations. These findings shed light on the complexity of Zn²⁺ storage on Ti₃C₂T_<em>x</em> MXene and provide a coherent mechanistic framework describing the transition from capacitive charge storage to zinc metal nucleation. Understanding and controlling this UPD-like regime offers opportunities for engineering MXene interfaces toward highly reversible Zn plating and advanced aqueous Zn-based energy-storage devices.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 18","pages":"12282–12293"},"PeriodicalIF":5.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067485","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"The Activating Effect of Carnallite and Hydrated MgCl2 on Hydrogen Absorption in Magnesium","authors":"Daniel Shtuckmeyster,&nbsp;Matvey Bereznitsky,&nbsp;Lonia Friedlander,&nbsp;Lee Shelly,&nbsp;Nitzan Maman,&nbsp;Ezra Hanuka,&nbsp;Nir Moskovich,&nbsp;Roni Z. Shneck,&nbsp;Isaac Jacob","doi":"10.1021/acsaem.6c02147","DOIUrl":"https://doi.org/10.1021/acsaem.6c02147","url":null,"abstract":"<p>We present activation strategies to enhance hydrogen absorption in magnesium. Magnesium chips, produced by mechanical chipping with a laboratory-scale milling device, were hydrogenated after adding activators and compared to pure Mg chips. It was found that following activation by turbomolecular evacuation at 300 °C for 3 h, MgCl₂·6H₂O-added Mg chips absorbed hydrogen at temperatures as low as 200 °C. Also, the addition of the activator eliminated the incubation period and improved the hydrogen absorption rate by a factor of three compared with pure Mg chips. These enhancements are attributed to the decomposition of MgCl₂·6H₂O during the activation process, which releases HCl gas. The HCl gas reacts with surface constituents on the Mg chips to form MgCl₂. This reaction is associated with breaking the oxide and carbonate layers, subsequently forming cracks and exposing an active surface. The modified surface chemistry promotes hydrogen dissociation and diffusion, thereby accelerating the first hydrogen absorption. Kinetic analysis of the first hydrogenation of activated Mg chips reveals that the process is governed by a low-dimensional nucleation and growth mechanism, like the mechanism taking place during the first hydrogen absorption in pure Mg chips. Application of the Avrami model further shows that the apparent activation energies for hydrogen absorption in activated Mg chips are lower than the values previously reported in the literature for pure Mg. This study highlights the benefits of adding small amounts, 4 wt % or less, of activator, which eliminates the incubation period, lowers the hydrogen absorption temperature, and increases the hydrogenation rate. These results demonstrate the potential of adding activators to produce highly reactive hydrogen storage materials.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 18","pages":"12510–12521"},"PeriodicalIF":5.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067511","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Rapid and Reversible Switching of Photoluminescence through Structural Dimensionality in Lead-Free Sb-Doped (CH3NH3)2NaInBr6 Double Perovskite","authors":"Parthapratim Nath,&nbsp;Pratap Vishnoi","doi":"10.1021/acsaem.6c01655","DOIUrl":"https://doi.org/10.1021/acsaem.6c01655","url":null,"abstract":"<p>Stimuli-responsive photoluminescent halide double perovskites present environmentally benign alternatives to lead-based systems for sensing and information encryption. Here, we report acetone-induced rapid transformation of a yellow-emissive (λ_em = 585 nm), one-dimensional (CH₃NH₃)₂NaInBr₆:Sb double perovskite to an orange-emissive (λ_em = 660 nm), zero-dimensional (CH₃NH₃)₄InBr₇:Sb compound. This structural and optical switching occurs within seconds and is reversible over multiple cycles. This study presents a rare example of solvatochromism in a hybrid In(III)-based halide double perovskite, significantly expanding the scope of this important class of materials for optical switching applications.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 18","pages":"12162–12168"},"PeriodicalIF":5.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067528","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Self-Polymerized Perfluorinated Iron Phthalocyanine/Carbon Nanotube Catalyst with Integrated Mass-Transport Channels for Efficient Oxygen Reduction","authors":"Mingjie Liu,&nbsp;Jian Wang,&nbsp;Linghong Li,&nbsp;Wei Ding,&nbsp;Weiyong Yuan,&nbsp;Zidong Wei,&nbsp;Jing He,&nbsp;Qinggang He","doi":"10.1021/acsaem.6c02242","DOIUrl":"https://doi.org/10.1021/acsaem.6c02242","url":null,"abstract":"<p>Fe–N–C single-atom catalysts are among the leading nonprecious-metal candidates for the oxygen reduction reaction (ORR) in fuel cells, but their performance in membrane electrode assemblies is constrained by poor active-site utilization and sluggish mass transport within the catalyst layer. These limitations arise, in part, because the high-temperature pyrolysis used to prepare Fe–N–C materials introduces structural heterogeneity, making it difficult to engineer porosity and surface chemistry without perturbing the active site. Here, we synthesized a perfluorinated iron phthalocyanine polymer catalyst (FePPCF₁₆/CNT) by self-polymerizing FePcF₁₆ monomers directly on carbon nanotube surfaces. The resulting macrocyclic polymer retains a well-defined Fe–N₄ coordination environment, as verified by X-ray absorption and photoelectron spectroscopy, while the CNT support withdraws electron density from the Fe center through π–π conjugation, shifting the iron oxidation state upward and decreasing the high-overpotential Tafel slope from &gt;160 to ∼91 mV dec⁻¹. The perfluorinated backbone renders the catalyst strongly hydrophobic (water contact angle: 128.2°), preventing liquid water from blocking gas pores while maintaining the water accessibility required for cathodic ORR. Concurrently, the interstitial voids and mesopores generated by CNT templating and polymerization create dedicated O₂ diffusion pathways, as confirmed by rapid bubble-uptake tests, while the interconnected pore network sustains OH^– conduction through the ionomer-filled interstices. In an operating anion exchange membrane fuel cell, FePPCF₁₆/CNT-0.75 delivers a half-wave potential of 0.90 V and a peak power density of 386 mW cm⁻², with negligible voltage loss in the mass-transport-limited regime above 200 mA cm⁻². These results demonstrate that self-polymerized macrocyclic catalysts can integrate electronic activation, ionic connectivity, and gas-transport pathways within a single material, without the structural heterogeneity introduced by pyrolysis.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 18","pages":"12534–12545"},"PeriodicalIF":5.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149071131","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Construction of Anion-Adsorbing UiO-67 Functionalized Polyimide Separator for Boosting Electrochemical Performance of Lithium-Metal Batteries","authors":"Jiaxuan Wang,&nbsp;Tongtong Zhang,&nbsp;Sibudjing Kawi,&nbsp;Yinhui Li","doi":"10.1021/acsaem.6c02350","DOIUrl":"https://doi.org/10.1021/acsaem.6c02350","url":null,"abstract":"<p>The development of high-energy-density lithium-metal batteries (LMBs) has imposed increasingly stringent requirements on the thermal stability, ionic conductivity, and interfacial compatibility of separators. To address the inherent drawbacks of conventional polypropylene (PP) separators, such as inadequate thermal stability and poor electrolyte wettability, a polyimide (PI) separator was fabricated via the nonsolvent induced phase separation (NIPS) method in this work. Furthermore, by introducing metal-organic framework (MOF) materials (UiO-67) into PI slurry, a PI/UiO-67 composite separator was successfully constructed, which achieves the synergistic optimization of the pore structure, surface morphology, and mechanical properties of the separator. The results demonstrate that the PI/UiO-67 composite separator retains the excellent thermal stability of the PI matrix, with no thermal shrinkage observed at 200 °C, while simultaneously exhibiting significantly improved electrode–electrolyte interfacial compatibility. Compared with the commercial PP separator (bulk resistance 2.97 Ω, interfacial impedance 165 Ω), the composite separator possesses a lower bulk resistance (2.28 Ω) and interfacial impedance(122 Ω). Additionally, integrating UiO-67 considerably improves the wettability of the electrolyte and the lithium-ion transference number (0.61) in the separator, which in turn markedly boosts the electrochemical stability and the long-cycle performance of LMBs. LMBs utilizing the PI/UiO-67 separator achieve a notable capacity retention of 87.4% after 150 cycles at a rate of 0.5 C. In tests conducted with lithium symmetric cells, stable cycling performance is observed for more than 600 h at a current density of 0.2 mA cm^–2. This study offers a valuable composite approach and theoretical insights for advancing the development of separators that ensure high safety and performance in LMBs.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 18","pages":"12587–12601"},"PeriodicalIF":5.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067486","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"AgNWs–PSS as a Passivating Interlayer Material with Local Nanowire Conduction for Silicon Solar Cells","authors":"Yonghui Chen,&nbsp;Xinyu Zhang,&nbsp;Zihao Liu,&nbsp;Chengchen Gong,&nbsp;Rong Wang,&nbsp;Jialiang Liu,&nbsp;Zilei Wang,&nbsp;Yujun Fu,&nbsp;Junshuai Li,&nbsp;Deyan He,&nbsp;Qiming Liu","doi":"10.1021/acsaem.6c02325","DOIUrl":"https://doi.org/10.1021/acsaem.6c02325","url":null,"abstract":"<p>The preparation of high-performance passivating interlayer materials with low-cost strategies is critically important for the development of silicon solar cells. Herein, a PSS/silver nanowire composite film (AgNWs–PSS) was synthesized by a solution-based method, which possesses superior electrical conductivity and passivation performance simultaneously. The conductivity of the film was optimized through the process of annealing, which resulted in a sheet resistance of approximately 40 Ω/□. At the optimal concentration (1 wt %), the minority carrier lifetime on the silicon surface was increased by approximately 3.3 times. The study shows that by adjusting the rotation speed to optimize film thickness and uniformity, the average photovoltaic conversion efficiency of the optimized devices reached 12.42 ± 1.1% (with a maximum efficiency of 13.5% for a single cell). In addition, efficiency improvements of at least 5% were observed at other concentrations.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 18","pages":"12546–12554"},"PeriodicalIF":5.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067565","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Probing of Strategic Disorder to Tune Thermoelectric Properties in Sb, Zn Co-doped Mg2Si0.3Sn0.7 through Extended X-ray Absorption Fine Structure Spectroscopy","authors":"Pritam Sarkar,&nbsp;Debdutta Lahiri,&nbsp;Debarati Das,&nbsp;Rajashri R. Urkude,&nbsp;Naveen Kumar Nagaraja,&nbsp;Shovit Bhattacharya,&nbsp;Nandini Garg,&nbsp;Vibha Saxena,&nbsp;Ajay Singh","doi":"10.1021/acsaem.6c01371","DOIUrl":"https://doi.org/10.1021/acsaem.6c01371","url":null,"abstract":"<p>Defect engineering in thermoelectric materials is a key approach for controlling lattice vibrations. Introducing defects in the lattice brings disorder, which facilitates scattering of phonons and suppresses heat transport. Although this can be beneficial for enhancing the material’s thermoelectric performance, increased disorder may also reduce charge carrier mobility, thereby lowering the electrical conductivity and overall thermoelectric efficiency. Therefore, optimizing the efficiency of thermoelectric materials requires careful management of the delicate interplay between structural order and disorder. In our recent work, controlled disorder was achieved in Mg₂(Si_0.3Sn_0.7)_0.98Sb_0.02 through Zn doping. This approach simultaneously enhanced carrier mobility (∼90 cm²/Vs) and weighted mobility (∼660 cm²/Vs) at 300 K while suppressing lattice thermal conductivity. In the present work, we investigate the nature of this disorder by employing a combination of experimental techniques including extended X-ray absorption fine structure (EXAFS), X-ray absorption near edge structure (XANES), positron annihilation lifetime spectroscopy (PALS), powder X-ray diffraction (XRD), and transmission electron microscopy (TEM). EXAFS analysis reveals that Zn occupies Mg-sites (Zn_S) and non-Mg (Zn_NS) sites in nearly equal proportions. XANES results confirm that Zn_NS sites promote p-d orbital hybridization, resulting in broader electronic bandwidth and enhanced charge transport. XRD and TEM analyses confirm that the dislocation density (N_D), predominantly associated with edge-type dislocations, increases monotonically with Zn doping, thereby enhancing phonon scattering. PALS measurements further support these findings by revealing the evolution of defects and the formation of vacancy clusters. Thus, controlled disorder provides an effective strategy for designing high performance thermoelectric materials.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 18","pages":"12234–12242"},"PeriodicalIF":5.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149067610","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Surfactant Doping Effect on the Performance of Gold Nanocluster-Modified Electrodes for CO2 Electroreduction","authors":"Michalina Zaborowska-Mazurkiewicz,&nbsp;Mostafa Torabi,&nbsp;Piotr Chyży,&nbsp;Izabela Pięta,&nbsp;Piotr Pięta,&nbsp;Renata Bilewicz","doi":"10.1021/acsaem.6c01963","DOIUrl":"https://doi.org/10.1021/acsaem.6c01963","url":null,"abstract":"<p>Electrochemical reduction of carbon dioxide (CO₂RR) is a promising approach for converting CO₂ into useful chemical products while helping to reduce atmospheric CO₂ levels. However, advancing this technology requires developing efficient electrocatalysts and precise surface engineering strategies to improve reaction selectivity, suppress competing reactions, and maximize active-site utilization. In this work, we modified highly oriented pyrolytic graphite (HOPG) electrodes with atomically precise Au₂₅(SC₄)₁₈ nanoclusters (AuNCs) mixed with didodecyldimethylammonium bromide (DDAB) surfactant using the Langmuir–Schaefer (LS) technique. This approach allowed us to control the arrangement of nanoclusters on the electrode surface by tuning the deposition surface pressure and the component ratios in the film. Adding DDAB to the AuNCs film: (i) improves the spreading of the AuNCs at the air–water and electrode–solution interfaces, enhancing the exposed active sites to the reactant, and (ii) provides a suitable hydrophobic microenvironment to increase local CO₂ concentration near the electrode. The electrode modified with an AuNCs film doped with 5% DDAB, in which AuNCs exposure and the hydrophobic effect of DDAB were optimally balanced, exhibited the best electrocatalytic activity toward CO₂. The maximum turnover frequency (TOF_CO) of 49.45 s^–1 at –1.50 V vs Ag|AgCl, achieved with the AuNCs/DDAB 95/5% electrode, was significantly higher than that of the electrode modified with AuNCs alone. These findings demonstrate that combining Au₂₅(SC₄)₁₈ nanoclusters with the positively charged DDAB surfactant provides an effective way to tune surface hydrophobicity, manipulate the microenvironment, and enhance nanocluster dispersion on the electrode.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"9 18","pages":"12395–12410"},"PeriodicalIF":5.5,"publicationDate":"2026-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149071140","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}