{"title":"Enhancing Fast-Charging Capability of Thick Electrode in Lithium-Ion Batteries Through Electronic/Ionic Hybrid Conductive Additive Engineering","authors":"Xiaoxue Chen, Renming Zhan, Zihe Chen, Xiancheng Wang, Shuibin Tu, Shiyu Liu, Yujie Zeng, Tiancheng Dong, Kai Cheng, Yangtao Ou, Yuchen Tan, Yongming Sun","doi":"10.1002/aenm.202500242","DOIUrl":"https://doi.org/10.1002/aenm.202500242","url":null,"abstract":"The attainment of lithium-ion batteries (LIBs) featuring high energy density necessitates the anode to exhibit substantial mass loading and thickness. However, this presents a formidable challenge for fast charging due to inferior Li-ion transport capability throughout the electrode depth, resulting in diminished capacity, reduced lifespan, and potential safety hazards. Here, an alternative strategy is put forth that utilizes an electronic/ionic hybrid conductive additive as a substitution for the conventional conductive reagent. This particular additive showcases carbon black (CB) particles adorned with ultrathin red phosphorus nanolayer (≈2 nm) (CB-P), which undergo in situ transformation into stable ultrathin lithium phosphide (Li<sub>3</sub>P) nanolayer-coated CB particles during the operation of the battery. Benefiting from the significant contribution of Li<sup>+</sup> conductive enhancement, the introduction of Li<sub>3</sub>P enables significantly increased apparent Li<sup>+</sup> transference number and similar ionic conductivity compared to CB additive (0.67 vs 0.42, 5.2 vs 4.1 mS cm<sup>−1</sup>). Notably, the pouch cell with graphite anode and CB-P additive demonstrates a high capacity filling ratio of 83.5% within 15 min (4C, relative to that at 0.5C) under a high anode loading of 14.4 mg cm<sup>−2</sup> (4.4 mAh cm<sup>−2</sup> at 0.5C). The full pouch cell with SiO<i><sub>x</sub></i> anode and CB-P additive exhibits an 82.1% capacity refilling at 4C charging rate (15 min, relative to that of 0.2C). In consideration of the superior compatibility with current electrode processing, the CB-P additive can serve as a direct replacement for traditional CB additives in existing batteries and boost the implementation of fast-charging LIBs with high energy density.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"36 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143737276","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kenza Elbouazzaoui, Andrii Mahun, Valeriia Shabikova, Laurent Rubatat, Kristina Edström, Jonas Mindemark, Daniel Brandell
{"title":"Enabling High-Voltage Polymer-Based Solid-State Batteries Through Reinforcements with LiAlO2 Fillers","authors":"Kenza Elbouazzaoui, Andrii Mahun, Valeriia Shabikova, Laurent Rubatat, Kristina Edström, Jonas Mindemark, Daniel Brandell","doi":"10.1002/aenm.202405249","DOIUrl":"https://doi.org/10.1002/aenm.202405249","url":null,"abstract":"Poor ionic conductivity, low Li<sup>+</sup> transference number, and limited electrochemical stability plague all-solid-state Li-metal batteries based on solid polymer electrolytes (SPEs). One strategy to overcome these hurdles is the insertion of ceramic fillers to generate composite polymer electrolytes (CPEs). These are based either on active (ion-conductive) fillers like Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> or passive (non-conductive) fillers like Al<sub>2</sub>O<sub>3.</sub> In this work, the effect of passive Li-containing fillers is showcased, exemplified by a CPE platform of poly(trimethylene carbonate) (PTMC:LiTFSI) with LiAlO<sub>2</sub> particles. The inclusion of such fillers shows a strikingly positive effect. The ionic conductivity is greatly improved by one order of magnitude at 20 wt% of LiAlO<sub>2</sub> compared to the pristine PTMC SPE. Moreover, the Li<sup>+</sup> transference number is significantly boosted and reaches values close to unity (<i>T</i>\u0000<sub>+</sub> = 0.97 at 20 wt% of LiAlO<sub>2</sub>), effectively rendering the material a single-ion conductor. The CPEs show outstanding cycling stability vs Li-metal, and electrochemical stability of up to 5 V vs Li<sup>+</sup>/Li. When implemented in a solid-state battery cell with LiNi<sub>0.33</sub>Mn<sub>0.33</sub>Co<sub>0.33</sub>O<sub>2</sub> (NMC111) and Li-metal, a stable cycling performance for over 100 cycles is observed. This demonstrates the potential of using microsized and cost-effective LiAlO<sub>2</sub> fillers in CPEs for applications in all-solid-state Li-metal batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"66 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143734281","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Synchronous Hetero-Interface and Vacancy Engineering for Construction of Pitaya-Like CoSe1-x/C@NC@ZnSe Nanosphere Toward Ultrastable Sodium-Ion Half/Full Batteries","authors":"Wenpei Kang, Mengjia Han, Mang Niu, Yazhan Liang, Ying Hu, Xiaoyu Fan, Xuguang An, Baojuan Xi, Daofeng Sun, Shenglin Xiong","doi":"10.1002/aenm.202500276","DOIUrl":"https://doi.org/10.1002/aenm.202500276","url":null,"abstract":"Transition metal selenides have attracted extensive attention as promising anode materials for sodium-ion batteries (SIBs) due to their fascinating physical chemistry characteristics. However, its cycling performance especially at high currents, is still unsatisfactory owing to the intrinsic limited conductivity. Herein, N-doped carbon shell coated and ZnSe bonded Se-vacancy enriched CoSe<sub>1-x</sub> (CoSe<sub>1-x</sub>/C@NC@ZnSe, CZSCV) nanospheres with abundant hetero-interfaces are designed through an in situ Se transfer strategy. Owing to the ingenious structure, as an anode material in SIBs, CZSCV demonstrates superior cycling stability (363.5 mAh g<sup>−1</sup> at 10 A g<sup>−1</sup> after 1000 cycles) and high-rate sodium storage capability (193.9 mAh g<sup>−1</sup> at 20 A g<sup>−1</sup> after 5000 cycles). Meanwhile, in the CZSCV//Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub>@C full cell, it also delivers a stable capacity of 201.4 mAh g<sup>−1</sup> at 1.0 A g<sup>−1</sup> and provides a high energy density of 397.4 Wh kg<sup>−1</sup> with a power density of 231.6 W kg<sup>−1</sup>. Based on the kinetics analysis and the density functional theory calculation, the hetero-interfaces and enriched Se-vacancies can synergistically accelerate the Na<sup>+</sup>/electron transfer, owing to the charge redistribution, the decreased diffusion barrier of Na<sup>+</sup> and increased pseudo-capacitive capacity contribution. As a result, excellent high-rate anode material can be achieved for the SIBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"17 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713658","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Biologically Insoluble Binder for High-Performance Cathodes in Lithium-Ion Batteries","authors":"Jinwei Zhou, Siyao Wu, Qihou Li, Feixiang Wu","doi":"10.1002/aenm.202406032","DOIUrl":"https://doi.org/10.1002/aenm.202406032","url":null,"abstract":"Binders are vital for maintaining the structural integrity and stability of electrodes in rechargeable batteries. The system of soluble polyvinylidene fluoride in N-methyl-2-pyrrolidone (NMP) is commonly used for commercial cathodes in Li-ion batteries. However, this system has remaining issues, including reliance on the toxic NMP solvent, weak van der Waals bonding, and obnoxious swelling in liquid organic electrolytes, causing difficulty in electrode manufacture and deterioration of mechanical properties during cycles. Herein, inspired by the artificial fishing bait, an eco-friendly and renewable wheat gluten (WG) derived from biomass wheat is utilized as a versatile insoluble binder for battery cathodes. Little water molecules can act as switches for adhesive properties of WG, demonstrating insoluble characteristics, robust hydrogen-bonding capabilities, and a uniform elastic network coating that serves as an effective artificial interphase on cathode materials. Additionally, this binder not only stabilizes the electrolyte by inhibiting and scavenging free radicals but also maintains its rigid mechanical properties in the electrolyte without swelling, resulting in a rather stable microenvironment for active particles, and demonstrating stable cycling performance over 500 cycles of various cathodes such as LiCoO<sub>2</sub>, LiNi<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub>, and LiFePO<sub>4</sub>. This bio-renewable, water-insoluble, and low-cost protein binder offers a promising pathway for advancing high-specific-energy cathode technologies.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"36 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723842","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Innovative Approach to Recycle Lithium-Ion Battery Electrolytes via Sequential Chemical Processes","authors":"Ting-Wei Hsu, Albert Lipson, Zhengcheng Zhang","doi":"10.1002/aenm.202500655","DOIUrl":"https://doi.org/10.1002/aenm.202500655","url":null,"abstract":"The rapid growth of electric vehicles (EV) has driven the widespread use of lithium-ion batteries (LIBs). This will result in a large amount of spent batteries that if not properly disposed will pose significant environmental damage, especially from the electrolyte. The electrolyte contains lithium hexafluorophosphate (LiPF<sub>6</sub>), which when treated by either incineration or water washing can generate harmful F- and P-containing substances such as hydrofluoric acid (HF). In this study, an innovative two-step process is presented to separate and purify both the solvents and lithium salts from the spent electrolyte. Antisolvent assisted precipitation is used to selectively isolate LiPF<sub>6</sub> salt in the form of a complex with ethylene carbonate. Subsequent distillation then separates the volatile electrolyte solvents and antisolvent from each other effectively. In addition, a new process to further purify LiPF<sub>6</sub> from its ethylene carbonate (EC) complex is also presented. This electrolyte recycling method not only enables the recovery of the high-value LiPF<sub>6</sub> salt and the electrolyte solvents, but also paves the way for environmentally responsible and circular LIB recycling.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"30 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713661","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hongbo Mo, Lian Wang, Yin Li, Tao Zhu, Aleksandr Sergeev, Jingbo Wang, Yanling He, Zhilin Ren, Atta Ur Rehman, Muhammad Umair Ali, Yueyang Wang, Dong-Keun Ki, Kam Sing Wong, Gang Li, Jasminka Popović, Aleksandra B. Djurišić
{"title":"Multifunctional Universal Additive for Stable and Efficient Inverted Perovskite Solar Cells","authors":"Hongbo Mo, Lian Wang, Yin Li, Tao Zhu, Aleksandr Sergeev, Jingbo Wang, Yanling He, Zhilin Ren, Atta Ur Rehman, Muhammad Umair Ali, Yueyang Wang, Dong-Keun Ki, Kam Sing Wong, Gang Li, Jasminka Popović, Aleksandra B. Djurišić","doi":"10.1002/aenm.202500088","DOIUrl":"https://doi.org/10.1002/aenm.202500088","url":null,"abstract":"The performance of perovskite solar cells has significantly improved over the years in part due to defect passivation in the bulk and at the interfaces. While many additive molecules have been reported in the literature, they are commonly applicable only to one particular perovskite composition. Here we investigate a multifunctional additive, 4-amino-5-bromo nicotinic acid (ABrNA), for use in both methylammonium (MA)-free perovskites with different Br content (bandgaps ranging from 1.53 to 1.73 eV) as well as MA-containing perovskites. Significant performance improvements are obtained for all compositions, which can be attributed to the presence of multiple functional groups capable of modifying the crystallization of the perovskite as well as passivating defects. Exceptional features of ABrNA make it a promising universal passivator, which leads to a PCE increase from 23.9% to 25.0% for CsFAMA solar cells, and from 22.0% to 23.0% for MA-free solar cells. The ABrNA passivated MA-free devices also exhibit exceptional operational stability, with T<sub>90</sub> exceeding 1000 h under ISOS-L-1 testing conditions. In addition, significant performance improvement is observed with ABrNA for modules in both conventional and inverted device architectures, further confirming the universality of ABrNA additive.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"3 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713659","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Lifecycle Synergistic Prelithiation Strategy of Both Anode and Cathode for High-Performance Lithium-Ion Batteries","authors":"Wei Zhong, Renjie He, Linfeng Peng, Wei Liu, Jiayue Peng, Haolin Zhu, Jingyu Xiang, Shijie Cheng, Jia Xie","doi":"10.1002/aenm.202406007","DOIUrl":"https://doi.org/10.1002/aenm.202406007","url":null,"abstract":"Prelithiation is recognized as an effective technology for addressing the depletion of active lithium, but conventional methods are constrained by their reliance on singular lithium replenishment mechanisms and limited functionality. Herein, a synergistic and comprehensive lifecycle prelithiation technology is introduced as applicable to both anode and cathode. For anode prelithiation, highly reactive biphenyl lithium is leveraged as a lithium replenishing agent, supplemented by functional additives, ethoxy(pentafluoro)cyclotriphosphazene (PFPN) and fluoroethylene carbonate (FEC), to generate a robust SEI enriched with Li<sub>3</sub>N, LiF, Li<sub>3</sub>P and Li<sub>2</sub>O. This approach not only compensates for the initial active lithium loss but also fortifies the structural integrity of the SEI. For cathode prelithiation, the high-capacity lithium replenisher Li<sub>2</sub>C<sub>2</sub>O<sub>4</sub> and Li<sub>2</sub>C<sub>4</sub>O<sub>4</sub> comprising B, N double-doped carbon loaded Mo<sub>2</sub>C-W<sub>2</sub>C (Mo-W@BNC) heterogeneous catalysts is employed, which exhibits superior catalytic performance in facilitating the release of lithium. The exceptional efficient liberations of lithium are achieved at discharge voltages of 3.78 V and 4.14 V for Li<sub>2</sub>C<sub>2</sub>O<sub>4</sub> and Li<sub>2</sub>C<sub>2</sub>O<sub>4</sub>, respectively. The prelithiation for both anode and cathode mitigates the initial active lithium loss by 22.6%. Moreover, a singular activation during subsequent usage contributes an additional 0.8 mAh cm<sup>−2</sup> of active lithium, achieving a capacity retention of 99.3% after 250 cycles at 0.5C.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"61 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703221","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hao Zhang, Zhibo Song, Kai Yang, Yundong Zhou, Yuchen Ji, Lu Wang, Yuxiang Huang, Shenyang Xu, Jianjun Fang, Wenguang Zhao, Guoyu Qian, Shanglin Wu, José V. Anguita, Gustavo F. Trindade, Shida Xue, Haoliang Wang, Ian S. Gilmore, Yan Zhao, Feng Pan
{"title":"In Situ Aminolysis of Fluoroethylene Carbonate Induced Low-Resistance Interphase Facilitating Extreme Fast Charging of Graphite Anodes","authors":"Hao Zhang, Zhibo Song, Kai Yang, Yundong Zhou, Yuchen Ji, Lu Wang, Yuxiang Huang, Shenyang Xu, Jianjun Fang, Wenguang Zhao, Guoyu Qian, Shanglin Wu, José V. Anguita, Gustavo F. Trindade, Shida Xue, Haoliang Wang, Ian S. Gilmore, Yan Zhao, Feng Pan","doi":"10.1002/aenm.202406104","DOIUrl":"https://doi.org/10.1002/aenm.202406104","url":null,"abstract":"Achieving extreme fast charging (XFC) lithium-ion batteries (LIBs) is essential for future battery applications, yet challenges remain in facilitating interfacial lithium-ion transportation across solid electrolyte interphase (SEI). While traditional SEI design prioritizes chemical composition, this study constructs an “ion-seepage” SEI framework accentuating the spatial distribution and arrangements of inorganic components via in-situ aminolysis reaction between fluoroethylene carbonate (FEC) and protic amines. This SEI architecture with tailored organic and nanoscale inorganic component distributions boosts interfacial Li<sup>+</sup> transfer kinetics, ultimately enabling XFC and stable low-temperature cycling. Practical validation at the pouch-cell level exhibits excellent high-rate (up to 10C) performance, highlighting the great potential of protic amines in commercial extreme fast-charging LIBs. Moreover, this strategy exhibits considerable versatility, across various protic amines, electrolyte systems, and anode materials, providing a universal approach for developing XFC batteries and valuable insights for SEI design.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"25 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703030","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jin-Hee Kim, Jae-Hwan Hyun, Sihyun Kim, Woo Hyun Park, Seung-Ho Yu
{"title":"Phosphorus-Based Flame-Retardant Electrolytes for Lithium Batteries","authors":"Jin-Hee Kim, Jae-Hwan Hyun, Sihyun Kim, Woo Hyun Park, Seung-Ho Yu","doi":"10.1002/aenm.202500587","DOIUrl":"https://doi.org/10.1002/aenm.202500587","url":null,"abstract":"The increasing demand for high-performance energy storage systems has driven a significant focus on developing electrolytes for lithium-ion batteries (LIBs), known for their high energy density and cycle stability. Organic electrolytes play a crucial role in enhancing battery performance due to their high ionic conductivity and wide electrochemical stability. However, their flammability and volatility pose serious safety risks, including thermal runaway and fire hazards. To address these issues, research is advancing on flame-retardant electrolytes, particularly fluorine (F)-based and phosphorus (P)-based compounds. F-based flame-retardants work by interrupting flame propagation through radical scavenging mechanisms but require high concentrations to be effective, leading to increased costs and adverse effects on electrolyte properties. In contrast, P-based flame-retardants offer distinct advantages, including lower toxicity, reduced smoke generation, and high thermal and chemical stability. These properties allow P-based additives to be effective at lower concentrations, minimizing their impact on cost and electrolyte performance. This review highlights the diverse structures of P-based flame-retardant additives, exploring their characteristics, mechanisms, and impacts on battery performance, while also proposing future directions for next-generation materials to improve the safety and stability of LIBs, paving the way for fire-resistant, high-performance energy storage solutions.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"99 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703031","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Feng Liu, Chunyang Zhang, Kejian Lu, Xueli Yan, Yi Wang, Dengwei Jing, Liejin Guo, Maochang Liu
{"title":"Pilot-Scale Photoreforming of Hydrolyzed Polylactic Acid Waste to High-Value Chemicals and H2 via Atomic Ru Integration","authors":"Feng Liu, Chunyang Zhang, Kejian Lu, Xueli Yan, Yi Wang, Dengwei Jing, Liejin Guo, Maochang Liu","doi":"10.1002/aenm.202500015","DOIUrl":"https://doi.org/10.1002/aenm.202500015","url":null,"abstract":"Photoreforming of polylactic acid (PLA) waste into valuable chemicals offers a promising approach for environmental protection and waste valorization, yet faces challenges of low yields and harsh conditions. Herein, a Cd<sub>0.5</sub>Zn<sub>0.5</sub>S nanotwin catalyst decorated with Ru single atoms and clusters is reported, enabling selective photoreforming of PLA into pyruvic acid (PA) and H<sub>2</sub>. It is demonstrated that Ru single atoms favor PA formation via hydroxyl dissociation, while the further incorporation of Ru clusters serve as active sites for H<sub>2</sub> production. This synergistic effect significantly enhances photocatalytic performance, achieving 96.8% PA selectivity and efficient H<sub>2</sub> production with a record-breaking apparent quantum efficiency of 83.7% at 400 nm. This approach is scalable for outdoor processes, utilizing direct 1 m<sup>2</sup> sunlight irradiation to deliver ≈1191 mL h<sup>−1</sup> of H<sub>2</sub> and 47.27 mmol h<sup>−1</sup> of PA from PLA waste, paving a viable pathway for large-scale simultaneous production of high-value chemicals and H<sub>2</sub>.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"58 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695219","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}