ACS Applied Energy Materials最新文献

{"title":"Light-Induced Phase Mixing as One Origin for the Degradation of Phase-Impure 2D Perovskite Solar Cells","authors":"Ying Jiang,&nbsp; and ,&nbsp;Xiaoming Zhao*,&nbsp;","doi":"10.1021/acsaem.5c0044010.1021/acsaem.5c00440","DOIUrl":"https://doi.org/10.1021/acsaem.5c00440https://doi.org/10.1021/acsaem.5c00440","url":null,"abstract":"<p >Quasi-two-dimensional perovskites have emerged as promising photovoltaic materials due to their remarkable stability compared to conventional 3D perovskites; however, their stability still falls short of the requirements for practical applications. Therefore, understanding the origins of intrinsic instability in 2D perovskite solar cells is essential for promoting their widespread use in optoelectronic technologies. Here, we studied the degradation of solar cells based on two kinds of 2D perovskite phases, aligned mix phase and pure phase, and found under light aging, the aligned mix phases gradually reverted to stoichiometric phases, indicative of light-induced phase mixing. During the aging process, the morphology of the perovskite thin films deteriorated, accompanied by an increase in the number of bulk-phase defects. To mitigate this phase mixing behavior, we employed larger-volume ligands to prepare 2D perovskites. The perovskite devices based on (OA)₂(FA)₃Pb₄I₁₃ demonstrated remarkable stability, maintaining 95% of their initial PCE after 4000 h of maximum power point tracking under one-sun illumination, representing one of the most stable quasi-2D perovskite solar cells to date.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 8","pages":"5414–5420 5414–5420"},"PeriodicalIF":5.4,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143878418","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":"Dual-Interface Engineering for Improved High-Voltage Performance in PEO-Based Solid-State Lithium-Metal Batteries","authors":"Zehui Zhang,&nbsp;Shuo Huang,&nbsp;Jianhe Hong,&nbsp;Xunzhi Miao and Hongyun Jin*,&nbsp;","doi":"10.1021/acsaem.4c0284810.1021/acsaem.4c02848","DOIUrl":"https://doi.org/10.1021/acsaem.4c02848https://doi.org/10.1021/acsaem.4c02848","url":null,"abstract":"<p >Poly(ethylene oxide) (PEO)-based solid electrolytes have attracted significant attention due to their high ionic conductivity, low expansion, and excellent compatibility with lithium-metal anodes. However, their oxidative stability is typically limited to below 3.9 V. This study addresses this limitation by forming a stable cathode–electrolyte interphase at the interface between the cathode and PEO-based composite polymer electrolyte (CPE), facilitated by the decomposition of the functional additive LiPO₂F₂ during cycling. Additionally, the incorporation of ethylene carbonate as a plasticizer significantly enhances the ionic conductivity. The parasitic reactions and lithium dendrite growth are effectively suppressed at the anode interface, allowing the Li/CPE/Li cell to achieve an outstanding lifespan of 2000 h at a current density of 0.1 mA cm^–2. Moreover, the oxidation voltage of the CPE reaches up to 4.82 V. The LiNi_0.33Co_0.33Mn_0.33O₂/CPE/Li cell demonstrates a high discharge capacity of 138.1 mAh g^–1 at a cutoff voltage of 4.2 V, maintaining an impressive capacity retention rate of 89.2% after 140 cycles.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 8","pages":"4983–4992 4983–4992"},"PeriodicalIF":5.4,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143878384","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":"Magnetic Stimuli-Guided Multiple Charge Transfer Pathways for Boosted Overall Water Splitting","authors":"Moumita Chandra,&nbsp;Peeyush Pandey,&nbsp;Alpana Sahu and Mohammad Qureshi*,&nbsp;","doi":"10.1021/acsaem.5c0081010.1021/acsaem.5c00810","DOIUrl":"https://doi.org/10.1021/acsaem.5c00810https://doi.org/10.1021/acsaem.5c00810","url":null,"abstract":"<p >Stimuli-driven electrochemical water splitting has emerged as a promising strategy to enhance the electrocatalytic efficiency for overall water splitting. In this context, a series of electrocatalysts─cobalt borophosphate (CoBP), Ni-doped cobalt borophosphate (NCBP), and Ag₂S-decorated NCBP (Ag₂S@NCBP)─have been rationally designed and synthesized via a sequential solvothermal and wet-chemical approach. The influence of an external magnetic field on borophosphate-based bifunctional electrocatalysts has been sparsely investigated, concentrating on reaction kinetics such as relaxation times and directional motion of electrolyte. The composite Ag₂S@NCBP demonstrates remarkable electrocatalytic performance, achieving overpotentials of 253 mV for the oxygen evolution reaction (OER) and 73 mV for the hydrogen evolution reaction (HER) under the influence of an external magnetic field. These results are attributed to the faster relaxation for processes involving interfacial charge transfer and a dynamically favorable flow pattern of electrolyte ions causing the easy accessibility of active sites at the electrode, quantified by the improved double-layer capacitance (<i>C</i>_dl) from 0.045 to 0.15 mF cm^–2. As a result, the reaction kinetics of electrodes for HER and the OER are enhanced as evidenced by low Tafel slopes of 74 mVdec^–1 (OER) and 72 mVdec^–1 (HER). Additionally, the bifunctional activity of Ag₂S@NCBP enables efficient overall water splitting with a low cell voltage of 1.54 V at 10 mA cm^–2, accompanied by excellent stability for up to 40 h. Therefore, controlling multiple charge transfer pathways by charge carrier relaxation times using an external magnetic field offers an alternate approach to optimizing water-splitting technologies for sustainable energy applications.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 8","pages":"5493–5501 5493–5501"},"PeriodicalIF":5.4,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143878182","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":"Raspberry-like Gold Nanoparticle-Decorated Titania Nanorods for Plasmon-Enhanced Photoelectrochemical Oxygen Evolution","authors":"Anisa Fitriani Rosyadi,&nbsp;Anh Ngoc Nguyen and Hyojong Yoo*,&nbsp;","doi":"10.1021/acsaem.5c0047410.1021/acsaem.5c00474","DOIUrl":"https://doi.org/10.1021/acsaem.5c00474https://doi.org/10.1021/acsaem.5c00474","url":null,"abstract":"<p >The development of efficient photoelectrochemical (PEC) water splitting systems for the oxygen evolution reaction is essential for realizing sustainable hydrogen fuel production. Among the various strategies for enhancing PEC cell performance, plasmonic nanostructures, particularly gold nanoparticles, have emerged as highly promising candidates for improving the efficiency of photoanodes. Herein, we report the fabrication of a photoanode architecture consisting of raspberry-like gold nanoparticles (Au RLNPs) incorporated into hydrothermally synthesized TiO₂ nanorod arrays on a fluorine-doped tin oxide substrate (Au RLNP/TiO₂||FTO) for PEC water splitting application. The Au RLNPs, synthesized via a facile, single-step solution-phase approach, exhibit a distinctive morphology that gives rise to a significantly red-shifted surface plasmon resonance, thereby enhancing visible light harvesting and promoting charge carrier generation. As a result, the Au RLNP/TiO₂||FTO photoanode demonstrates a remarkable photocurrent density of 2.18 mA·cm^–2 at 1.23 V_RHE under AM 1.5G illumination. These findings underscore the substantial potential of the unique photoanode architecture for advancing the development of high-performance PEC water splitting systems.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 8","pages":"5431–5441 5431–5441"},"PeriodicalIF":5.4,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143878273","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":"Engineering NiRu Nanoalloys on N-Doped Carbon Nanocages for Efficient Electrocatalytic Hydrogen Oxidation Reaction","authors":"Na Jin,&nbsp;Xiao Yang,&nbsp;Yong Li,&nbsp;Wanjing Lai,&nbsp;Hailin Jiang,&nbsp;Yanghua Li,&nbsp;Kuo Liu,&nbsp;Yimeng Cai,&nbsp;Linjie Zhang* and Lili Han*,&nbsp;","doi":"10.1021/acsaem.5c0025910.1021/acsaem.5c00259","DOIUrl":"https://doi.org/10.1021/acsaem.5c00259https://doi.org/10.1021/acsaem.5c00259","url":null,"abstract":"<p >Hydrogen, characterized by its high energy density, efficiency, and environmentally benign output, emerges as a promising alternative to fossil fuels. However, the development of robust hydrogen oxidation reaction (HOR) catalysts for efficient energy conversion remains a significant challenge. Herein, a NiRu nanoalloy catalyst supported on N-doped hollow carbon nanocages (NiRu/NC) is synthesized via a tandem pyrolysis method. The NiRu/NC catalyst exhibits superior alkaline HOR activity, achieving diffusion-limited current density of 2.56 mA cm^–2 and maintaining stability for 80,000 s with a decay rate of only 5.9%, compared to a 28.7% decay rate for benchmark Pt/C after 35,000 s. Additionally, it demonstrates remarkable resistance to CO poisoning, with the current density decreasing by only 50.7% after 1800 s, while the current density of Pt/C dropped to 0 after 800 s. Density functional theory calculations indicate that Ni in the NiRu nanoalloy effectively modulates the electron distribution, thereby ameliorating the electronic structure and enhancing the adsorption of reaction intermediates. These optimizations endow NiRu/NC with both favorable hydrogen-binding energy (HBE) and hydroxyl-binding energy (OHBE), leading to improved HOR efficiency. This work not only offers an innovative approach for synthesizing high-performance alloy-based HOR catalysts but also deepens the fundamental understanding of the bimetallic synergistic mechanisms in HOR catalysis.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 8","pages":"5299–5308 5299–5308"},"PeriodicalIF":5.4,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143878179","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":"Achievable Surface–Bulk Structure Dual Reinforced by Room-Temperature Al-Induced Engineering Enables Stable Battery Cycling of 4.6 V LiCoO2","authors":"Zhengde Wang,&nbsp;Zhengfeng Zhang,&nbsp;Xingkai Zhang*,&nbsp;Rupeng Li,&nbsp;Yunxia Wang*,&nbsp;Jin Li and Bin Zhang*,&nbsp;","doi":"10.1021/acsaem.4c0329710.1021/acsaem.4c03297","DOIUrl":"https://doi.org/10.1021/acsaem.4c03297https://doi.org/10.1021/acsaem.4c03297","url":null,"abstract":"<p >The LiCoO₂ cathode cannot maintain stable battery cycling under high voltage, as the undesired release of lattice O and harmful surface side reactions compromise its structural stability, resulting in battery capacity degradation. Herein, inspired by architectural engineering, we proposed a surface–bulk structure dual-reinforced strategy to tackle the aforementioned challenges by room-temperature Al-induced engineering, which could achieve surface disordering and phosphating and bulk gradient Ni doping of the LiCoO₂ cathode. Such a multifunctional structure could delay the detrimental transition, restrain lattice O loss, reduce harmful surface side reactions, and form a phosphate-rich CEI with high ionic conductivity and stability. The as-prepared modified LiCoO₂ as the cathode in lithium-ion batteries displayed remarkably enhanced cycle stability than bare LiCoO₂ (91.9% vs 45.3% after 100 cycles in 3.0–4.6 V at a current density of 1 C). Even at a 5 C high rate, the modified LiCoO₂ cathode also displayed superb battery cycling (92% after 100 cycles at 3.0–4.6 V). This room-temperature Al-induced engineering is universal to other layered cathode materials.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 8","pages":"5082–5091 5082–5091"},"PeriodicalIF":5.4,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143878180","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":"Sodium Oleate-Modified Tin Oxide Electron Transport Layer for High-Performance Perovskite Solar Cells","authors":"Li Chen,&nbsp;Peng Li,&nbsp;Xin Liu,&nbsp;Shuxia Li,&nbsp;Liping Yang,&nbsp;Ning Kang* and Chenglong Wang*,&nbsp;","doi":"10.1021/acsaem.5c0017610.1021/acsaem.5c00176","DOIUrl":"https://doi.org/10.1021/acsaem.5c00176https://doi.org/10.1021/acsaem.5c00176","url":null,"abstract":"<p >Internal and surface defects in the tin oxide (SnO₂) electron transport layer (ETL) affect the performance of perovskite solar cells (PSCs). Herein, an effective strategy is designed to modify these defects for high-performance PSCs by incorporating sodium oleate (NaOA) into the SnO₂ ETL. The as-prepared SnO₂ + NaOA layer provides multiple nucleation sites to assist in the growth of the perovskite film with high crystal quality, increasing the charge transport capacity and suppressing nonradiative recombination. A champion power conversion efficiency (PCE) of up to 17.62% is obtained for PSCs with SnO₂ + NaOA ETL, corresponding to a filling factor (FF) of 76.00%, an open-circuit voltage (<i>V</i>_OC) of 1.104 V, and a short-circuit current density (<i>J</i>_SC) of 21.00 mA/cm². Besides, this device maintains an initial PCE of 86.17% in nitrogen for 30 days, compared with only 82.02% for the control device. Finally, it is found that the enhancement of <i>J</i>_SC can be attributed to the long-chain alkyl groups, and −COO^– and Na⁺ play a key role in boosting <i>V</i>_OC and FF. This work provides a promising strategy to optimize ETLs using amphiphilic surfactants for high-performance devices.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 8","pages":"5222–5229 5222–5229"},"PeriodicalIF":5.4,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143878181","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 Application of MgO in Janus Fibrous Membranes Enabling Efficient Radiative and Evaporative Cooling","authors":"Yefei Feng,&nbsp;Wangshu Tong*,&nbsp;Shengqian Wang,&nbsp;Bingwei Chen and Yihe Zhang*,&nbsp;","doi":"10.1021/acsaem.5c0064210.1021/acsaem.5c00642","DOIUrl":"https://doi.org/10.1021/acsaem.5c00642https://doi.org/10.1021/acsaem.5c00642","url":null,"abstract":"<p >Passive radiative cooling presents an energy-efficient thermal management strategy requiring zero external energy input, yet conventional hydrophobic cooling membranes often trap sweat and impurities at the skin interface, diminishing comfort and cooling efficacy. To overcome this limitation, we developed an electrospun dual-layer Janus fiber membrane with asymmetric wettability that synergistically combines passive radiative cooling with directional moisture transport. The Janus architecture facilitates continuous wicking of perspiration from the skin to the environment through its wettability gradient, significantly improving thermal regulation. Magnesium oxide (MgO) nanoparticles were strategically incorporated into the poly(vinylidene fluoride-<i>co</i>-hexafluoropropylene) (PVDF-HFP) layer, leveraging their exceptional phononic and electronic properties to achieve outstanding optical performance. The optimized membrane exhibits an average solar reflectance of 94.07% across 0.3–2.5 μm and high infrared emissivity of 90.03% in the atmospheric transparency window (8–13 μm). Outdoor evaluations demonstrated superior cooling performance compared to conventional cotton textiles, with the MgO@PVDF-HFP-PAN Janus membrane achieving an average temperature reduction of 8.7 °C and maximum cooling of 11.6 °C. Evaporative cooling experiments revealed sustained surface temperatures of 22.3 °C for the Janus membrane versus 31.6 °C for cotton, with evaporation contributing an additional 6.2 °C cooling enhancement. By integrating passive radiative cooling with evaporative cooling, this system effectively regulates heat dissipation and moisture transport, thereby enhancing thermal comfort across diverse environmental conditions.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 8","pages":"5482–5492 5482–5492"},"PeriodicalIF":5.4,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143878272","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":"Selective Loading of a Cobalt Species Cocatalyst on an Oxygen-Evolution Photocatalyst in a Silver-Inserted Z-Scheme System Consisting of Bismuth Vanadium Oxide and Zinc Rhodium Oxide for Enhanced Overall Water Splitting and Carbon Dioxide Reduction","authors":"Hiroshi Irie*,&nbsp;Masaomi Yoda,&nbsp;Toshihiro Takashima and Hiroshi Miyashita,&nbsp;","doi":"10.1021/acsaem.5c0038410.1021/acsaem.5c00384","DOIUrl":"https://doi.org/10.1021/acsaem.5c00384https://doi.org/10.1021/acsaem.5c00384","url":null,"abstract":"<p >We selectively loaded various amounts of a cobalt species (CoO<i>_<i>x</i></i>) cocatalyst for oxygen (O₂) evolution on bismuth vanadium oxide (Bi₄V₂O₁₁ (BVO)) as an O₂-evolution photocatalyst in a solid-state photocatalyst, a silver (Ag)-inserted BVO and zinc rhodium oxide (ZnRh₂O₄ (ZRO)) photocatalyst (BVO/Ag/ZRO (BAZ)), to form CoO<i>_<i>x</i></i>/BAZ. The amount of loaded CoO<i>_<i>x</i></i> was controlled by changing the photodeposition time to obtain CoO<i>_<i>x</i></i>/BAZ with up to 0.039 wt % Co vs BAZ. All the prepared CoO<i>_<i>x</i></i>/BAZ photocatalysts achieved overall water splitting irradiated with red light at a 700 nm wavelength, enhancing the hydrogen (H₂) and O₂ evolutions from water at a ratio of 2:1 compared with bare BAZ. Moreover, the apparent quantum efficiency (AQE) increased up to 0.11% under 700 nm-wavelength light irradiation. CoO<i>_<i>x</i></i> was demonstrated to function as a cocatalyst enhancing the overall water-splitting activity. It was confirmed that the CoO<i>_<i>x</i></i>/BAZ photocatalyst reduced carbon dioxide (CO₂) to methane (CH₄) and carbon monoxide (CO) and oxidize water to O₂ using water as an electron donor and proton source under 700 nm-wavelength light. In addition, copper (Cu) was selectively photodeposited as a H₂-evolution cocatalyst on ZRO, a H₂-evolution photocatalyst, in CoO<i>_<i>x</i></i>/BAZ to form CoO<i>_<i>x</i></i>/BAZ/Cu. CoO<i>_<i>x</i></i>/BAZ/Cu further enhanced the water-splitting activity with an AQE of 0.22% under 700 nm-wavelength light irradiation. Moreover, CoO<i>_<i>x</i></i>/BAZ/Cu reduced CO₂ and oxidized water to produce CH₄ and O₂, without producing CO, under 700 nm-wavelength light irradiation. Cu was confirmed to function as a cocatalyst for enhancing the overall water-splitting reaction and CO₂ reduction to selectively generate CH₄.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 8","pages":"5370–5377 5370–5377"},"PeriodicalIF":5.4,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143878407","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":"In Situ Growth of α-MoC Nanoparticles on Bamboo-Structured Carbon Nanotubes as Proton-Feeding Centers of the Fe Site, Achieving Efficient Oxygen Reduction Reaction in Multiple Environments","authors":"Xianchang Cui,&nbsp;Fei He*,&nbsp;Yumeng Zhang,&nbsp;Yijun Gao,&nbsp;Shanshan Song,&nbsp;Linbo Cao,&nbsp;Xiao Zhang* and Piaoping Yang*,&nbsp;","doi":"10.1021/acsaem.5c0019110.1021/acsaem.5c00191","DOIUrl":"https://doi.org/10.1021/acsaem.5c00191https://doi.org/10.1021/acsaem.5c00191","url":null,"abstract":"<p >Oxygen reduction reaction (ORR) is a key component of the next generation energy storage system, and most of the current research on ORR catalysts focuses on promoting the rapid conversion process of oxygen-containing intermediates, but its reaction kinetics is also severely limited by the laborious and slow proto-coupled electron transfer (PCET) process. Therefore, it is imperative to develop a high-performance ORR catalyst that can simultaneously accelerate the rapid conversion of PCET and oxygen-containing intermediates. In this context, we purposely grew α-MoC nanoparticles (Fe-MoC@NCNT) in situ on Fe and N codoped bamboo-structured carbon nanotubes to realize the simultaneous promotion of rapid conversion of oxygen intermediates and PCET process. According to the theoretical study, the adjacent α-MoC nanoparticles accelerate the dissociation of water and can act as the proton supply center of Fe–N₄ active site to promote the PCET process, while the oxygenated intermediates can achieve rapid transformation in the Fe–N₄ active site in order to reduce the reaction barrier of the, ORR. Due to the synergistic effect of Fe–N₄ active site and α-MoC, Fe-MoC@NCNT exhibits excellent ORR properties in both alkaline and neutral environments with half-wave potentials of 0.895 and 0.744 V, respectively. Using Fe-MoC@NCNT as the negative catalyst, the assembled aluminum-air battery has a high-power peak rate density of 285.7 mW cm^–2. This work elucidates the method of constructing adjacent proton-supplying centers to optimize the ORR kinetics of single atomic sites and proposes ideas for the synthesis of low-cost and excellent performance ORR catalysts.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"8 8","pages":"5239–5250 5239–5250"},"PeriodicalIF":5.4,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143878406","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}