Advanced Energy Materials最新文献

Effects of Tail States in Cs2AgBiBr6 Double Perovskites on Solar Cell Performance: A Temperature-Dependent Study of Photovoltaic External Quantum Efficiency, Open-Circuit Voltage, and Luminescence Cs2AgBiBr6双钙钛矿尾态对太阳能电池性能的影响：光伏外量子效率、开路电压和发光的温度依赖性研究

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-05-03 DOI: 10.1002/aenm.202500758

Firouzeh Ebadi, Kazem Meraji, Miguel A. Torre Cachafeiro, Florian Wolf, Maximillian T. Sirtl, Thomas Bein, Wolfgang Tress

{"title":"Effects of Tail States in Cs2AgBiBr6 Double Perovskites on Solar Cell Performance: A Temperature-Dependent Study of Photovoltaic External Quantum Efficiency, Open-Circuit Voltage, and Luminescence","authors":"Firouzeh Ebadi, Kazem Meraji, Miguel A. Torre Cachafeiro, Florian Wolf, Maximillian T. Sirtl, Thomas Bein, Wolfgang Tress","doi":"10.1002/aenm.202500758","DOIUrl":"https://doi.org/10.1002/aenm.202500758","url":null,"abstract":"Cs2AgBiBr6 double perovskites have been investigated as a lead-free alternatives to lead-based perovskites. However, despite promising features such as high luminescence lifetimes, solar-cell efficiencies and the open-circuit voltage still remain too low. Various spectroscopic studies suggested multiple reasons such as a fast relaxation into localized self-trapped excitonic and polaronic states. However, it remains unclear to what extent the suggested processes are the culprit for the low device performance. In this study, full devices are characterized as a function of temperature, focusing on highly sensitive measurements of tail states. In the spectral response, a strongly-temperature-dependent Urbach energy is identified, indicative of high dynamic disorder. The current generated from the excitonic absorption becomes only limiting at lower temperatures with an activation energy of 0.15 eV. Analysis of light-, temperature- and voltage-dependent photoluminescence (PL) indicates that charge extraction correlates with PL quenching and PL does not originate from geminate pairs. The bandgap deduced from temperature-dependent open-circuit voltage is found at 2.0 eV, coinciding with the PL peak. In contrast, tail-state excitation leads to lower open-circuit voltage and luminescence that cannot be quenched with voltage. Having identified the importance of tail-state features, the methodology might assist in optimizing materials and devices for enhanced efficiency.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"8 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-05-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143901708","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}

引用次数: 0

Molecular Bridging of Buried Interface Flattens Grain Boundary Grooves and Imparts Stress Relaxation for Performance Enhancement and UV Stability in Perovskite Solar Cells 在钙钛矿太阳能电池中，埋藏界面的分子桥接使晶界沟槽平坦，并赋予应力松弛以提高性能和紫外线稳定性

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-05-03 DOI: 10.1002/aenm.202501296

Wei Cheng, Peng Huang, Zhijie Gao, Yansheng Chen, Linying Ren, Qingguo Feng, Xiaodong Liu, Shahzada Ahmad, Zuowan Zhou

{"title":"Molecular Bridging of Buried Interface Flattens Grain Boundary Grooves and Imparts Stress Relaxation for Performance Enhancement and UV Stability in Perovskite Solar Cells","authors":"Wei Cheng, Peng Huang, Zhijie Gao, Yansheng Chen, Linying Ren, Qingguo Feng, Xiaodong Liu, Shahzada Ahmad, Zuowan Zhou","doi":"10.1002/aenm.202501296","DOIUrl":"https://doi.org/10.1002/aenm.202501296","url":null,"abstract":"The limitations imposed by interfacial voids and residual stress fundamentally constrain the stability and performance ceiling of perovskite solar cells (PSCs). Herein, the study engineers a molecular bridge by the placement of ectoine (Ec) at the SnO2/perovskite interface. The experimental investigations coupled with first-principles density functional theory (DFT) calculations reveal that the carboxyl group preferentially passivates uncoordinated Sn4+ defects and oxygen vacancies in SnO2, while the imine group establishes robust coordination with Pb2⁺ ions in the perovskite to passivate uncoordinated Pb2+ defects. The bi-anchoring molecular bridging mechanism facilitates the residual stress release, flattens the grain boundary grooves, and significantly suppresses the nonradiative recombination. In turn, the Ec-modified PSCs achieve a power conversion efficiency (PCE) of 24.68% (vs 22.56% for control). Significantly, the unencapsulated PSCs with the Ec show improved UV stability, retaining 80.12% of the initial PCE after 130 h (equivalent to 1412 h of solar irradiation) under 365 nm ultraviolet irradiation (50 mW cm−2). The study uncovers the role of Ec as a molecular bridge to optimize the buried interface for effective yet stable solar cell fabrication.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"18 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-05-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143901707","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}

引用次数: 0

Deciphering the Synergy of Multiple Vacancies in High-Entropy Layered Double Hydroxides for Efficient Oxygen Electrocatalysis 破译高熵层状双氢氧化物中多个空位的协同作用，用于高效氧电催化

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-05-02 DOI: 10.1002/aenm.202502065

Yiyue Zhai, Xiangrong Ren, Tao Gan, Liaona She, Qingjun Guo, Na Yang, Bolun Wang, Yao Yao, Shengzhong (Frank) Liu

{"title":"Deciphering the Synergy of Multiple Vacancies in High-Entropy Layered Double Hydroxides for Efficient Oxygen Electrocatalysis","authors":"Yiyue Zhai, Xiangrong Ren, Tao Gan, Liaona She, Qingjun Guo, Na Yang, Bolun Wang, Yao Yao, Shengzhong (Frank) Liu","doi":"10.1002/aenm.202502065","DOIUrl":"https://doi.org/10.1002/aenm.202502065","url":null,"abstract":"Layered double hydroxides (LDHs) hold the promise of designing efficient and long-lived electrocatalysts for alkaline oxygen evolution reaction (OER), yet control of their activity and durability at ampere-scale current densities remains a challenge. Here, a high-entropy LDH anode integrating multiple metal and oxygen vacancies is reported that achieves superior and robust OER under industrial conditions. The molar ratio of Ni:Cr:Co:Zn:Fe in high-entropy LDHs engineers the electronic structure via the cocktail effect, yielding more high-valent metal ions that promote the electrochemical restructuring. Using various operando characterizations, the generation of γ-NiOOH active-phase on a high-entropy LDH surface is identified, triggering the oxygen-vacancy-site mechanism (OVSM). Importantly, a volcano relationship is found between intrinsic OER activity (overpotential value) and the local coordination structure of Ni active centers (matching with the ΔG*OH). The integration of multiple metal and oxygen vacancies significantly optimizes the adsorption-free energy of oxygen-containing intermediates that are anchored at Ni active sites, boosting the OVSM. Accordingly, the developed Ni0.15Cr0.15Co0.4Zn0.1Fe0.2-LDH@NF achieves 1 A·cm−2 at 1.81 V and enables stable operation over 300 h in anion exchange membrane water electrolyzer. These findings elucidate the synergistic effects of multiple vacancies in high-entropy LDH electrocatalysts and enlighten the vacancy engineering for designing high-efficiency OER catalysts.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"21 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143897666","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}

引用次数: 0

Structural Design and Interface Modification with Selective H+ Binding of 3D Zinc Anode for Aqueous Zinc-Ion Batteries 水性锌离子电池三维锌阳极的结构设计与界面修饰

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-05-02 DOI: 10.1002/aenm.202500785

Ming Lu, Bo-Hao Xiao, Yong-Xia Lu, Kang Xiao, Zhao-Qing Liu

{"title":"Structural Design and Interface Modification with Selective H+ Binding of 3D Zinc Anode for Aqueous Zinc-Ion Batteries","authors":"Ming Lu, Bo-Hao Xiao, Yong-Xia Lu, Kang Xiao, Zhao-Qing Liu","doi":"10.1002/aenm.202500785","DOIUrl":"https://doi.org/10.1002/aenm.202500785","url":null,"abstract":"The reversible cycling lifespan of zinc-ion batteries is fundamentally compromised by the hydrogen evolution reaction (HER) and the growth of Zn dendrites induced by tips on 2D zinc metal anodes. Herein, a 3D zinc metal alloy anode to effectively mitigate dendrite growth and HER through dual regulation of the interface is presented. Experimental results confirm that the second component with strong H+ adsorption can efficiently inhibit Hads desorption diffusion, thereby suppressing HER. Moreover, the robust interaction between the in-situ derived solid electrolyte interphase (SEI) layer and Zn2+ also enhances Zn2+ diffusion kinetics, reduces nucleation energy barriers, achieving dendrite-free deposition of Zn2+. The as-prepared 3D Zn-W anodes achieve a lifespan of up to 2400 h with a coulombic efficiency of 99.23% achieved in symmetrical cells and can also exceed 200 h when operated at a depth of discharge as high as 91.46%. This work provides a simple and effective approach toward enhancing the safety and efficiency of zinc-ion batteries while significantly improving Zn utilization efficiency.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"35 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143897667","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}

引用次数: 0

Harnessing Renewable Energy via Tunable Hydrovoltaic Power Generation on Cobalt Intercalated Nitrogen-doped Graphene 利用钴插层氮掺杂石墨烯可调谐水力发电利用可再生能源

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-05-02 DOI: 10.1002/aenm.202500138

Subhabrata Das, Monika, Shahjad Ali, Daya Rani, Harini EM, Pooja Bhardwaj, Shumile Ahmed Siddiqui, Mohd Afshan, Seema Rani, Nikita Chaudhary, Soumyadip Sharangi, Jyoti, Ehesan Ali, Goutam sheet, Kaushik Ghosh

{"title":"Harnessing Renewable Energy via Tunable Hydrovoltaic Power Generation on Cobalt Intercalated Nitrogen-doped Graphene","authors":"Subhabrata Das, Monika, Shahjad Ali, Daya Rani, Harini EM, Pooja Bhardwaj, Shumile Ahmed Siddiqui, Mohd Afshan, Seema Rani, Nikita Chaudhary, Soumyadip Sharangi, Jyoti, Ehesan Ali, Goutam sheet, Kaushik Ghosh","doi":"10.1002/aenm.202500138","DOIUrl":"https://doi.org/10.1002/aenm.202500138","url":null,"abstract":"With the increasing demand and rising environmental adulteration, researchers are exploring sustainable energy harvesting methods. Water-based energy harvesting using carbonaceous matrices and 2D layered materials has gained significant attention due to their superior electrical properties at low-dimension. This study demonstrates cobalt-nitrogen-doped graphene (Co-N-Gr) thin layers are presented as an efficient medium for harvesting energy from diverse water sources, including simulated seawater (0.6m NaCl), rainwater, and for differentiating pH levels and detecting acidic contaminants (H2SO4 and HNO3) in the aquatic environment. The nitrogen-functionalized graphene-assisted cobalt immobilization enhances power generation by ≈108 times compared to pristine graphene (P-Gr) without any secondary heterojunction materials. The Co-N-Gr matrix improves hydrophilicity, facilitating ionic interaction and charge transfer, achieving ≈2.7 nW power generation under drop-by-drop motion of DI water. A mechanistic understanding is developed through experimental findings supported by density functional theory calculation to identify the role of anionic (Cl− and F−) interaction via electrical double-layer formation. The selective higher interaction energy with HNO3 leads to four times higher power generation than H2SO4 at the same concentration, highlighting its potential for the integration of renewable energy harvesting along with rain quality detection onto a single platform for developing commercialized smart windows.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"39 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143897574","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}

引用次数: 0

Rational Design of Molecular Passivator to Mitigate Surface Defects and Stabilize Organic Cation in Perovskite Photovoltaics 合理设计分子钝化剂以减轻钙钛矿光伏中表面缺陷和稳定有机阳离子

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-05-02 DOI: 10.1002/aenm.202500389

Yehui Wen, Tianchi Zhang, Xingtao Wang, Weihua Ning, Yong Wang, Deren Yang

{"title":"Rational Design of Molecular Passivator to Mitigate Surface Defects and Stabilize Organic Cation in Perovskite Photovoltaics","authors":"Yehui Wen, Tianchi Zhang, Xingtao Wang, Weihua Ning, Yong Wang, Deren Yang","doi":"10.1002/aenm.202500389","DOIUrl":"https://doi.org/10.1002/aenm.202500389","url":null,"abstract":"Pure iodide FA-based perovskites are one of the most promising light-absorbing materials for photovoltaics (PVs). However, high-density surface defects and unstable organic components within the FA-based perovskites not only reduce efficiency but also compromise operational stability. Herein, a rational molecular design strategy is reported to optimize the electronic structure and steric hindrance of pyrazine-based passivated molecules, enabling stable FA-based perovskite PVs. Both theoretical and experimental results reveal that pyrazine can effectively passivate positive charge defects, though its efficacy is limited by low electron cloud density and insufficient steric hindrance. The introduction of methyl groups in the pyrazine ring can effectively fine-tune the electronic structure and spatial properties of the passivated molecules. Full substitution of the hydrogen atoms on pyrazine with trimethyl groups achieves an optimal balance between electronic modulation and steric effects. The optimized pyrazine-based passivated molecule exhibits significantly improved defects passivation effect by enhancing binding affinity between the pyrazine ring and the perovskite, while simultaneously stabilizing FA+ cation through strengthening hydrogen bonding. Finally, the optimized FA-based device demonstrates an efficiency of 25.93%, and the unencapsulated devices retain 94% of their initial efficiency after 1000 h maximum power point tests in the nitrogen atmosphere at 25 °C.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"9 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143897582","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}

引用次数: 0

Form Factor–Free Magneto-Triboelectric Generator for Standalone Power Line IoT Applications 用于独立电力线物联网应用的无形状因数磁摩擦发电机

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-05-02 DOI: 10.1002/aenm.202500856

Hyun Soo Kim, Min Hyuk Lee, Do-Heon Kim, Dong-Gyu Lee, Iman M. Imani, SungHoon Hur, Young Joon Ko, Yeong Uk Choi, Hyunah Cho, So-Min Song, Tae Kyoung Yoon, In Woo Oh, Jong Hoon Jung, Jun Chen, Yunseok Kim, Heemin Kang, Jungho Ryu, Jeong Min Baik, Hyun-Cheol Song

{"title":"Form Factor–Free Magneto-Triboelectric Generator for Standalone Power Line IoT Applications","authors":"Hyun Soo Kim, Min Hyuk Lee, Do-Heon Kim, Dong-Gyu Lee, Iman M. Imani, SungHoon Hur, Young Joon Ko, Yeong Uk Choi, Hyunah Cho, So-Min Song, Tae Kyoung Yoon, In Woo Oh, Jong Hoon Jung, Jun Chen, Yunseok Kim, Heemin Kang, Jungho Ryu, Jeong Min Baik, Hyun-Cheol Song","doi":"10.1002/aenm.202500856","DOIUrl":"https://doi.org/10.1002/aenm.202500856","url":null,"abstract":"The growing reliance on electronic devices has made ambient magnetic field harvesting a promising solution for powering low-power, small-scale technologies, such as those used in the Internet of Things (IoT). While metal alloy-based magneto-deformation materials have traditionally been used to capture energy from stray magnetic fields, they are costly and lack versatility. To advance magnetic field harvesting, it is essential to develop cost-effective, high-performance, and adaptable magneto-deformation materials. Incorporating ferromagnetic metal powders into polymers can induce magneto-rheological behavior. This quasi-solid magneto-rheological effect enables the generation of mechanical vibrations in response to an oscillating external magnetic field. Here, a functional composite film is presented that achieves efficient and straightforward magneto-deformation by integrating Fe powder with poly(vinylidene fluoride-trifluoroethylene). To further enhance the performance of the composite film, MoS2–SiO2 core–shell nanoparticles is exploited for improved charge trapping and employ ferroelectrics to increase the contact potential difference (CPD). The composite film shows a bending displacement of 1 mm in a 4 Oe magnetic field, with each magneto-triboelectric module generating 14.28 mW. The four fabricated modules successfully harvest real-time energy from the stray magnetic field of an electric pot, enabling a battery-free Bluetooth IoT sensor.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"14 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143897664","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}

引用次数: 0

In Situ Polymerized Localized High-Concentration Electrolytes for Ultrahigh-Rate Sodium Metal Batteries 超高倍率钠金属电池的原位聚合局部高浓度电解质

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-05-02 DOI: 10.1002/aenm.202500887

Xue Wang, Yuzhou Bai, Zhuoran Lv, Yuan Liu, Wujie Dong, Hui Bi, Fuqiang Huang

{"title":"In Situ Polymerized Localized High-Concentration Electrolytes for Ultrahigh-Rate Sodium Metal Batteries","authors":"Xue Wang, Yuzhou Bai, Zhuoran Lv, Yuan Liu, Wujie Dong, Hui Bi, Fuqiang Huang","doi":"10.1002/aenm.202500887","DOIUrl":"https://doi.org/10.1002/aenm.202500887","url":null,"abstract":"Sodium metal batteries (SMBs) offer a promising alternative to lithium-ion systems due to the natural abundance of sodium. Nevertheless, their practical application is hindered by challenges of sodium dendrite growth and unstable electrolyte/electrode interfaces in conventional liquid electrolytes. Here, an in situ polymerized localized high-concentration gel electrolyte (IS-LHCE) is presented and engineered through strategic integration of 1,3-dioxolane as both diluent and polymer precursor. Unlike conventional approaches using inert diluents, the design establishes a polymer-confined solvation structure that simultaneously achieves anion coordination regulation and ion transport decoupling. This unique configuration reduces Na+ activation energy to 0.0379 eV, enabling exceptional ionic conductivity of 6.07 × 10−4 S cm−1 and a wide electrochemical stability window (≈4.56 V). The in situ formed polymer network of IS-LHCE promotes preferential anion decomposition, forming a gradient inorganic-rich solid electrolyte interphase dominated by NaF/Na2S phases, which enables Na||Na symmetric batteries to achieve unprecedented cycling stability of over 1,200 h at 0.1 mA cm−2. The Na3V2(PO4)3||Na full batteries demonstrate record-breaking longevity, with 90.8% capacity retention after 3,000 cycles at 10 C rate. This work presents a new paradigm in polymer electrolyte design, fundamentally resolving the longstanding trade-offs between interfacial instability and ion transport, avoiding dendrite formation, and advances practical high-energy-density SMBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"276 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143897573","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}

引用次数: 0

Optimization of Adsorption Sites for Selective Hydrobenzoin and Syngas Production in a Single Photoredox Cycle 单次光氧化还原循环中选择性苯并苯甲酸酯和合成气吸附位点的优化

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-05-02 DOI: 10.1002/aenm.202500950

Jian Lei, Hongyuan Yang, Bo Weng, Yu-Ming Zheng, Shifu Chen, Prashanth W. Menezes, Sugang Meng

{"title":"Optimization of Adsorption Sites for Selective Hydrobenzoin and Syngas Production in a Single Photoredox Cycle","authors":"Jian Lei, Hongyuan Yang, Bo Weng, Yu-Ming Zheng, Shifu Chen, Prashanth W. Menezes, Sugang Meng","doi":"10.1002/aenm.202500950","DOIUrl":"https://doi.org/10.1002/aenm.202500950","url":null,"abstract":"Integrating benzyl alcohol oxidation with carbon dioxide (CO2) reduction in a single photoredox catalysis is of high economic and practical interest. However, it remains challenging to controllably regulate the selectivity of specific C─C coupling chemicals (oxidation products) and the ratio of carbon monoxide and hydrogen (CO/H2) for syngas (reduction products). Herein, an efficient photocatalyst consisting of CdS nanorods decorated by Ni2P (NP/CdS) is developed, which achieves remarkable performance, producing C─C coupling hydrobenzoin (HB) with an excellent yield of ≈315.4 µmol g−1 h−1 and selectivity of ≈90%. This performance originates from the optimized adsorption of benzaldehydes and protons, promoting the generation of the critical radical intermediates (•CH(OH)Ph). Meanwhile, the favorable desorption of •CH(OH)Ph and HB from the binding sites is attained. On the other hand, by increasing the Ni2P content in NP/CdS, the CO/H2 ratio can be adjusted across a wide range (from ≈15:1 to ≈2.6:1), enabling syngas compositions suitable for industrial feedstock applications. This tunability is attributed to the lower CO2 affinity of the Ni2P phase compared to CdS while demonstrating higher activity for H2 evolution. This work presents a novel approach for selectively and efficiently producing HB and tunable syngas simultaneously.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"40 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143897665","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}

引用次数: 0

Layered-to-Layered Synthesis of High-Performance Nickel-Rich Layered Cathodes via Low-Temperature Oxidation of Layered Hydroxide Precursor 层状氢氧前驱体低温氧化制备高性能富镍层状阴极

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-05-02 DOI: 10.1002/aenm.202500325

Hang Li, Li Wang, Jinkun Wang, Zhibei Liu, Aimin Du, Xiangming He

{"title":"Layered-to-Layered Synthesis of High-Performance Nickel-Rich Layered Cathodes via Low-Temperature Oxidation of Layered Hydroxide Precursor","authors":"Hang Li, Li Wang, Jinkun Wang, Zhibei Liu, Aimin Du, Xiangming He","doi":"10.1002/aenm.202500325","DOIUrl":"https://doi.org/10.1002/aenm.202500325","url":null,"abstract":"Nickel-rich layered transition metal oxide cathodes, such as LiNixCoyMnzO2 (LiTMO2), are set to revolutionize the capabilities of lithium-ion batteries with their exceptional energy density. The conventional synthesis method, which entails high-temperature sintering of MO6-structured hydroxide precursors, leads to the decomposition of the MO6 framework to form rock salt. Although it can be reconstituted after lithiation to form a layered structure, structural defects typically remain in the final product. Hereby, a two-step, low-temperature oxidation, and lithiation process is introduced, where the MO6 structure remains, thereby producing outstanding cathode materials. The Ni0.9Co0.05Mn0.05(OH)2 precursor is initially oxidized at ambient temperature to Ni0.9Co0.05Mn0.05OOH, followed by lithiation below 90 °C. The resulting material exhibits an impressive discharge capacity of over 239.3 mAh g−1 at 0.1C within 2.7–4.3 V, and an initial coulombic efficiency (ICE) of 95.76%. A subsequent high-temperature treatment significantly enhances crystallinity, further improving the material's discharge capacity, ICE, rate capability, and cycling stability, surpassing those of traditionally sintered materials. This approach is further applied to the synthesis of LiNi0.825Co0.115Mn0.06O2 and LiNiO2, demonstrating its versatility in synthesizing nickel-rich materials. Additionally, this method helps optimize nickel-rich LiTMO2 performance while mitigating initial irreversible reactions.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"18 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143897669","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}

引用次数: 0