物理化学学报最新文献

{"title":"Applications of generative artificial intelligence in battery research: Current status and prospects","authors":"Hengrui Zhang,&nbsp;Xijun Xu,&nbsp;Xun-Lu Li,&nbsp;Xiangwen Gao","doi":"10.1016/j.actphy.2025.100115","DOIUrl":"10.1016/j.actphy.2025.100115","url":null,"abstract":"<div><div>With the rapid development of renewable energy and electric vehicles, batteries, as the core components of electrochemical energy storage systems, have become a global focus in both scientific research and industrial sectors due to their critical impact on system efficiency and safety. However, the complex multi-physics reactions within batteries make traditional mathematical models inadequate for comprehensively revealing their mechanisms. The key to solving this problem lies in introducing data-driven approaches, which have laid a solid foundation for battery research and development through extensive accumulation of experimental data and extraction of effective information. Generative artificial intelligence (GAI), leveraging its powerful latent pattern learning and data generation capabilities, has already found widespread applications in protein structure prediction, material inverse design, and data augmentation, demonstrating its broad application prospects. Applying GAI to battery research workflows with diverse battery data resources could provide innovative solutions to challenges in battery research. In this perspective, we introduce the core principles and latest advancements of generative models (GMs), including Generative Adversarial Network (GAN), Variational Auto-Encoder (VAE), and Diffusion Model (DM), which can learn the latent distribution of the input samples to generate new data by sampling from it. Applications of GAI in battery research are then reviewed. For battery materials design, by learning material compositions, structures, and properties, GM can generate novel candidate materials with desired properties through conditional constraints, significantly extending the chemical space to be explored. For electrode microstructure characterization, GM can serve as a bridge for interconversion and integration of different image data, enhance the quality of microscopic characterization, and generate realistic synthetic data. For battery state estimation, GM can perform data augmentation and feature extraction on battery datasets, which benefits the model performance for battery state estimation. Lastly, we discuss the challenges and future development directions in terms of data governance and model design, including data quality and diversity, data standardization and sharing, usability of synthetic data, interpretability of GM, and foundational models for battery research. For the innovation and advancement of battery technology, this perspective offers theoretical references and practical guidelines for implementing GAI as an effective tool in battery research workflows by discussing its status and prospects in this field.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 10","pages":"Article 100115"},"PeriodicalIF":10.8,"publicationDate":"2025-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144472367","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Challenges and prospects of photocatalytic H2O2 production","authors":"Mahmoud Sayed ,&nbsp;Han Li ,&nbsp;Chuanbiao Bie","doi":"10.1016/j.actphy.2025.100117","DOIUrl":"10.1016/j.actphy.2025.100117","url":null,"abstract":"<div><div>Hydrogen peroxide (H₂O₂) is one of the 100 most important chemicals used extensively in bleaching, disinfection, and synthetic chemistry industries. It is currently used as a fuel in direct fuel cells. The current H₂O₂ production relies on the harsh anthraquinone oxidation approach. Photocatalytic H₂O₂ production is a more favorable alternative from environmental, sustainability, and economic viewpoints. The process requires water and molecular oxygen as inputs and sunlight as the sole power source. Despite these merits, the practical application of this technology remains challenging. The most common bottlenecks are the photocatalyst's inadequacy, uphill thermodynamics, sluggish process kinetics, and competitive and backward reactions. This paper discusses these limitations and highlights the proposed perspectives to improve the efficiency and selectivity, aiming to pave the way toward large-scale H₂O₂ photogeneration.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100117"},"PeriodicalIF":10.8,"publicationDate":"2025-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144279508","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Research progress of transient absorption spectroscopy in solar energy conversion and utilization","authors":"Fengying Zhang ,&nbsp;Yanglin Mei ,&nbsp;Yuman Jiang ,&nbsp;Shenshen Zheng ,&nbsp;Kaibo Zheng ,&nbsp;Ying Zhou","doi":"10.1016/j.actphy.2025.100118","DOIUrl":"10.1016/j.actphy.2025.100118","url":null,"abstract":"<div><div>With the development of ultrafast laser technology, time-resolved spectroscopy has become an essential tool to study the microscopic photophysical mechanisms on ultrafast time scales in the field of solar energy conversion and utilization. Transient absorption spectroscopy (TAS), as an essential technology for studying photoinduced ultrafast electron transfer and photo-induced carrier dynamics, has the unique advantage of revealing key dynamic processes, such as the generation, separation, transport, and recombination of photogenerated carriers. Focusing on light-to-chemical and light-to-electrical energy conversion, this review summarizes TAS applications in two primary solar energy conversion systems: photocatalysis and solar cells. Firstly, according to the different requirements of photocatalysis (emphasizing migration for surface reactions) and solar cells (highlighting interfacial carrier separation efficiency), we summarize design strategies and recent advances for enhancing carrier utilization from three perspectives: electron manipulation, hole manipulation and surface interfacial processes. Subsequently, special attention is given to how <em>in situ</em> spectroscopy elucidates the influence mechanisms of microscopic energy conversion processes and device performance under complex application scenarios involving photo-electro-thermal couplings. Finally, the forward-looking development direction of basic research in solar energy conversion and utilization is summarized, which provides theoretical support for rational design and performance optimization of solar energy conversion materials, reactions, and devices.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100118"},"PeriodicalIF":10.8,"publicationDate":"2025-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144279509","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Integrating high surface area and electric conductivity in activated carbon by in-situ formation of a less-defective carbon network during selective chemical etching","authors":"Jing Zhang ,&nbsp;Su Zhang ,&nbsp;Qiqi Li ,&nbsp;Linken Ji ,&nbsp;Yutong Li ,&nbsp;Yukang Ren ,&nbsp;Xiaobei Zang ,&nbsp;Ning Cao ,&nbsp;Han Hu ,&nbsp;Peng Liang ,&nbsp;Zhuangjun Fan","doi":"10.1016/j.actphy.2025.100114","DOIUrl":"10.1016/j.actphy.2025.100114","url":null,"abstract":"<div><div>Activated carbons are widely used as electrode materials for supercapacitors owing to their large surface area, good electric conductivity, and outstanding electrochemical stability. Improving the electric conductivity of activated carbon is crucial for promoting its electrochemical energy storage, but it is hard to achieve because well-developed pores usually break the continuous conductive network. To solve this problem, researchers have developed several methods, such as the selection of highly-conjugated carbon precursors, high-temperature post-treatment, compositing with highly conductive nanocarbons, and local catalytic graphitization. However, these methods generally suffer from high cost, low efficiency, and the sacrifice of specific surface area. Herein, we propose a selective chemical etching strategy to prepare activated carbon with both high surface area and electric conductivity using a mixture of pitch and polyacrylonitrile (PAN) as the precursor. Through systematic investigation of the activation behavior of pure pitch, pure PAN, and the composite precursors, we demonstrate that the PAN-derived carbon contains amorphous and crystallized components. During activation, the amorphous carbon is primarily etched away due to its high reactivity, leading to the in-situ formation of less-defective carbon as the entire conductive network. The optimized sample shows a surface area of 2773 m² g⁻¹ and 2.6 times increased electric conductivity of 912 S m⁻¹, outperforming most of the reported activated carbons. Furthermore, the strong cross-linking between pitch and PAN molecules through pre-oxidation leads to a higher activated carbon yield of 58 % than the pure pitch activated carbon (34 %). The optimized cross-linking structure also allows the activator K⁺ to be adsorbed more easily in the carbon precursor, which enhances the activation efficiency. As a result, the embedded PAN simultaneously constructs a conductive network and promotes activation efficiency, leading to the integration of high electric conductivity and surface area of the activated carbon. For aqueous supercapacitor application, at the high electrode mass loading of 10 mg cm⁻², the optimized material shows remarkable areal capacitance (2.8 F cm⁻² at 1 A g⁻¹) and good rate performance (41 % retention at 50 A g⁻¹). The corresponding device shows high energy densities (10.9 Wh·kg⁻¹) and remarkable cycle stability (100 % retention after 50000 cycles). The reason is that good electric conductivity enables high surface area utilization, significantly improved electric double-layer formation and ion transport kinetics. This work demonstrates the significant potential of highly conductive activated carbon for practical applications and provides novel insights into the design of conductive activated carbon for advanced energy storage.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 10","pages":"Article 100114"},"PeriodicalIF":10.8,"publicationDate":"2025-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144298269","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enhanced sodium storage performance of asphalt-derived hard carbon through intramolecular oxidation for high-performance sodium-ion batteries","authors":"Wenhui Li ,&nbsp;Yakun Tang ,&nbsp;Yusheng Zhou ,&nbsp;Yue Zhang ,&nbsp;Wenhai Zhang ,&nbsp;Qingtao Ma ,&nbsp;Lang Liu ,&nbsp;Sen Dong ,&nbsp;Yuliang Cao","doi":"10.1016/j.actphy.2025.100119","DOIUrl":"10.1016/j.actphy.2025.100119","url":null,"abstract":"<div><div>The development of high-performance and low-cost hard carbon plays a crucial role in the commercialization of sodium-ion batteries (SIBs). Asphalt is considered a suitable hard carbon precursor due to its wide distribution, abundance, and cost-effectiveness. However, its low capacity and poor electrochemical reaction kinetics limit its further application. Herein, we have successfully synthesized asphalt-based hard carbon nanosheets through a process of intramolecular oxidation, facilitated by the synergistic action of mixed acids. The introduction of sulfuric acid plays a crucial role in expanding the tightly packed asphalt molecules, which in turn allows for the intramolecular oxidation of asphalt molecules by nitric acid. This oxidation process effectively introduces oxygen-containing functional groups (OFGs), leading to an increase in interlayer spacing and the formation of a more nanoporous structure, resulting in both enhanced capacity and improved rate performance. The optimized asphalt-based hard carbon boosts reversible capacity from 115.0 to 304.4 mAh∙g⁻¹ at 0.03 A g⁻¹, and the plateau capacity is increased by 5.5 times. This work provides a profound understanding of the impact of liquid-phase acid oxidation on the structure and composition of sodium-storage hard carbon, and further unveils an effective method for obtaining low-cost and high-performance asphalt-based hard carbon.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 10","pages":"Article 100119"},"PeriodicalIF":10.8,"publicationDate":"2025-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144308135","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Membrane-anchoring nanoengineered carbon dots as a pyroptosis amplifier for robust tumor photodynamic-immunotherapy","authors":"Tiejin Chen ,&nbsp;Xiaokuang Xue ,&nbsp;Jian Li ,&nbsp;Minhui Cui ,&nbsp;Yongliang Hao ,&nbsp;Mianqi Xue ,&nbsp;Haihua Xiao ,&nbsp;Jiechao Ge ,&nbsp;Pengfei Wang","doi":"10.1016/j.actphy.2025.100113","DOIUrl":"10.1016/j.actphy.2025.100113","url":null,"abstract":"<div><div>Photodynamic therapy (PDT), as a FDA-approved therapeutic modality, has witnessed substantial advancements in the field of oncology. However, the conventional PDT may suffer poor prognosis due to the transient nature of ROS, excessive phototoxicity, and inducing traditional apoptosis. In this study, a nanoengineered carbon dots (NCDs) was constructed through electrostatic interaction between a positive-charged carbon dots photosensitizers (PCDs) and new indocyanine green (IR820). The introduction of IR820 at variable ratios could change the surface charge and amphiphilic characteristics of NCDs, thereby modulating the membrane-anchoring capability of NCDs. Besides, the J-aggregation of IR820 led to a redshift of fluorescence from NIR-I to NIR-II region, thereby achieving NIR-II imaging. Furthermore, the photoactivity of PCDs was quenched by IR820, with subsequent restoration of PDT occurring contingent on the photobleaching of IR820 <em>via</em> 750 nm laser irradiation. Finally, both <em>in vitro</em> and <em>in vivo</em> studies had demonstrated that under a cascaded laser irradiation, the membrane-targeted NCDs could effectively induce cell pyroptosis, thereby eradicating tumors with minimal side effects while simultaneously activating immune responses to inhibit tumor lung metastasis. This study developed a multifunctional nanoengieering carbon dots and offered novel perspectives for tumor photodynamic-immunotherapy with enhanced controllability, improved efficacy and high security.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 10","pages":"Article 100113"},"PeriodicalIF":10.8,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144307587","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Bandgap and adsorption engineering of carbon dots/TiO2 S-scheme heterojunctions for enhanced photocatalytic CO2 methanation","authors":"Wenlong Wang ,&nbsp;Wentao Hao ,&nbsp;Lang He ,&nbsp;Jia Qiao ,&nbsp;Ning Li ,&nbsp;Chaoqiu Chen ,&nbsp;Yong Qin","doi":"10.1016/j.actphy.2025.100116","DOIUrl":"10.1016/j.actphy.2025.100116","url":null,"abstract":"<div><div>S-scheme heterojunctions have garnered significant interest in photocatalytic CO₂ conversion to valuable products (e.g., CH₄) due to their enhanced charge separation and robust redox capabilities. Carbon dots (CDs), with their tunable band structures and light absorption ranges, show particular promise in constructing efficient S-scheme photocatalytic systems. Nevertheless, the critical roles of CDs' band alignment and surface adsorption properties in determining heterojunction configuration, charge carrier kinetics, and ultimately CO₂ activation/product selectivity distribution remain insufficiently explored. Herein, we construct four CDs/TiO₂ heterojunctions using CDs synthesized from varied carbon sources, in which S-scheme heterojunctions were successfully constructed based on cost-effective coal pitch (C-GQDs, 1.75 nm), glucose (G-CQDs, 1.84 nm), and acetone (CQDs-X, 1.82 nm) carbon sources, whereas Type-I heterojunctions were formed by carbon black based CDs (GQDs-A, 1.92 nm). Systematic investigations reveal that both the band structure and adsorption characteristics of CDs play important roles in the charge transfer path and separation efficiency, CO₂ adsorption and activation capacities, and product selectivity in photocatalytic CO₂ reduction. Remarkably, the introduction of CDs significantly broadens the photo-response range compared to fresh TiO₂, and in particular, the C-GQDs/TiO₂ exhibits exceptional performance with a CH₄ production rate of 32.7 μmol·g⁻¹·h⁻¹, surpassing TiO₂ by 6.3-fold and outperforming GQDs-A/TiO₂, CQDs-X/TiO₂, and G-CQDs/TiO₂ by factors of 3.8, 2.7, and 2.3, respectively. This heterojunction simultaneously achieves 72.6 % CH₄ selectivity and 98.1 % hydrocarbons selectivity (encompassing CH₄, C₂H₆, C₂H₄, and C₃H₈). In contrast, composites incorporating GQDs-A, CQDs-X, or G-CQDs exhibit substantially diminished CH₄ selectivity (&lt;40.0 %). The high CH₄ production rate and selectivity of C-GQDs/TiO₂ can be attributed to its unique S-scheme heterojunction structure, higher reduction potential, and well-matched CO₂ and H₂O adsorption and activation capabilities. This study provides unique insights into the efficient photoreduction of CO₂ to CH₄ driven by the S-scheme heterojunction electron transfer pathway in CDs/TiO₂ photocatalysts.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100116"},"PeriodicalIF":10.8,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144279475","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Design of noble metal catalysts and reactors for the electrosynthesis of hydrogen peroxide","authors":"Kangjuan Cheng ,&nbsp;Chunxiao Liu ,&nbsp;Youpeng Wang ,&nbsp;Qiu Jiang ,&nbsp;Tingting Zheng ,&nbsp;Xu Li ,&nbsp;Chuan Xia","doi":"10.1016/j.actphy.2025.100112","DOIUrl":"10.1016/j.actphy.2025.100112","url":null,"abstract":"<div><div>Hydrogen peroxide (H₂O₂) is an eco-friendly oxidant vital for chemical synthesis, water treatment, and disinfection. However, the conventional anthraquinone production method is energy-intensive, generates waste, and requires hazardous transport of concentrated H₂O₂. Electrochemical H₂O₂ synthesis <em>via</em> a two-electron oxygen reduction reaction (2e⁻ ORR) has emerged as a sustainable alternative, enabling renewable-powered, decentralized production under mild conditions. Noble metal catalysts outperform alternatives in acidic media, demonstrating superior stability and selectivity. Despite these advantages, several technical challenges must be addressed to enable industrial-scale implementation. The primary challenge lies in optimizing catalyst performance to achieve both high activity and selectivity for the 2e⁻ pathway while suppressing the competing 4e⁻ pathway that produces water. This requires precise control of the catalyst’s electronic and surface structures. Additionally, the development of cost-effective reactor systems that can maintain high performance at scale presents another significant hurdle. Current research focuses on improving mass transport, current distribution, and product separation while minimizing energy consumption.</div><div>This review provides a comprehensive examination of recent progress in the 2e⁻ ORR, with particular emphasis on noble metal catalysts and reactor engineering. We begin by discussing the fundamental principles and reaction mechanisms underlying the 2e⁻ ORR, emphasizing the role of material design in optimizing catalytic performance. Noble-metal catalysts are categorized into four types, namely, pure metals, alloys, compounds, and single-atom catalysts, with a critical evaluation of their performance based on theoretical and experimental findings. The second part of the review focuses on reactor design strategies for practical applications. We evaluate reactor designs, including H-cells, flow cells, membrane electrode assemblies, and solid-state electrolyte cells, with a focus on their mass transport and scalability characteristics. Particular emphasis is placed on gas diffusion electrodes for improved oxygen accessibility and innovative <em>in situ</em> product separation methods. Finally, we discuss the remaining challenges and future directions, including the need for reduced noble metal loading, improved long-term stability, and system integration with renewable energy sources. The review concludes by highlighting the tremendous potential of electrochemical H₂O₂ production to transform industrial oxidation processes while contributing to the development of sustainable chemical manufacturing.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 10","pages":"Article 100112"},"PeriodicalIF":10.8,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144364490","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Rationally assembling different surface functionalized carbon dots for enhanced near-infrared tumor photothermal therapy","authors":"Xue Wu ,&nbsp;Yupeng Liu ,&nbsp;Bingzhe Wang ,&nbsp;Lingyun Li ,&nbsp;Zhenjian Li ,&nbsp;Qingcheng Wang ,&nbsp;Quansheng Cheng ,&nbsp;Guichuan Xing ,&nbsp;Songnan Qu","doi":"10.1016/j.actphy.2025.100109","DOIUrl":"10.1016/j.actphy.2025.100109","url":null,"abstract":"<div><div>Carbon dots (CDs) have emerged as promising photothermal agents for near-infrared (NIR)-mediated tumor therapy due to their excellent biocompatibility and tunable optical properties. However, it is still unclear how to precisely control their assembly behavior to enhance NIR absorption and photothermal conversion efficiency. In this work, we present a hyper-assembled electron donor/acceptor CDs complex (S-d/a-CDs), constructed by integrating electron-donating CDs (d-CDs) with electron-withdrawing CDs (a-CDs). This configuration significantly enhances the NIR absorption capacity of S-d/a-CDs. Under 740 nm laser irradiation, S-d/a-CDs achieve a remarkable photothermal conversion efficiency (PTCE) of 65.8 %. S-d/a-CDs exhibit negligible cytotoxicity and effective tumor accumulation capacity through intravenous administration, enabling complete tumor elimination after NIR laser irradiation. To our knowledge, this study is the first to exploit synergistic assembles of two types of CDs for photo-physical property engineering, establishing a groundbreaking paradigm for the development of advanced NIR-triggered photothermal materials.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100109"},"PeriodicalIF":10.8,"publicationDate":"2025-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144270331","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"The role of hydroxyl species in the alkaline hydrogen evolution reaction over transition metal surfaces","authors":"Ruizhi Duan ,&nbsp;Xiaomei Wang ,&nbsp;Panwang Zhou ,&nbsp;Yang Liu ,&nbsp;Can Li","doi":"10.1016/j.actphy.2025.100111","DOIUrl":"10.1016/j.actphy.2025.100111","url":null,"abstract":"<div><div>Understanding the activity-determining factors governing the alkaline hydrogen evolution reaction (HER) on transition metal catalysts is indispensable for water electrolysis with renewable energy. However, it remains a critical challenge. Although hydroxyl adsorption has been proposed to influence alkaline HER performance, its exact mechanistic role and quantitative correlations remain elusive. Here, we systematically investigate the alkaline HER on ten transition metal surfaces using density functional theory (DFT), revealing that hydroxyl adsorption critically modulates both pathway selection and reaction energy barrier. However, hydroxyl adsorption energy alone cannot fully explain the anomalous activity of certain catalysts, especially Pt. To address this, we introduce a multi-parameter coupled descriptor (ECS) that integrates electron occupancy (E), adsorption configuration (C), and surface crystallographic (S), enabling a qualitative evaluation of catalytic activity. This descriptor successfully elucidates previously unexplained activity trends and demonstrates a good correlation with over 10 experimental datasets, including those involving single-atom alloy (SAA) catalysts, indicating its robustness beyond pure metals. Our findings provide a descriptor based on the key species of hydroxyl for rational catalyst design and screening, and offer a fundamental framework for advancing the development of high-performance alkaline HER catalysts.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 9","pages":"Article 100111"},"PeriodicalIF":10.8,"publicationDate":"2025-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144270419","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}