Abstract: The electrochemical interfacial interaction of electrode materials with liquid electrolytes in electro-chemical energy storage systems including supercapacitors, metal ion batteries, and metal-based batteries have become a research hotspot and play a decisive role in electrochemical energy storage in terms of charging and discharging reaction principles of the electrode materials. However, there is still a long way from maturity due to the challenges related to the unsatisfactory electrolyte-philicity of electrode materials. In the last 20 years, several studies have been directed at discovering strategies to improve the electrolyte-philicity of electrode materials, optimizing the electrochemical interfacial interaction of the electrode materials with liquid electrolytes and exploring the relationship between electrolyte-philicity and electrochemical energy storage performance in the charging and discharging processes of the electrode materials. Unfortunately, the systematic and in-depth understanding of electrolyte-philicity of electrode materials has not been grasped in electrochemical energy storage systems. In this review, we highlight the fundamental scientific understanding of electrolyte-philicity of electrode materials and the relationship among electrolyte-philicity and electrochemical energy storage performance of electrode materials. The definition of electrolyte-philicity of electrode materials is first proposed based on the interaction between the electrode material and electrolyte ions as the essence of electrochemical energy storage of the electrode materials. More important, how the electrolyte-philicity of electrode materials optimizes the electrochemical energy storage performance of the electrode materials has been expounded from the rapid and effective contact of the electrode materials with electrolyte ions under uncharged state to electrochemical interfacial interaction between the electrode materials and electrolytes under the charged state. Then, the fundamental physical and chemical interactions so that the electrode materials may be electrolyte-philic are summarized, and the mechanisms of improving the electrolyte-philicity of electrode materials by surface modification are illustrated based on those interactions. Finally, the future perspectives for important areas of electrolyte[1]philicity of electrode materials are presented.
赵磊博士(Dr. Lei Zhao)：2019年至今，在兰州理工大学材料科学与工程学院（有色金属先进加工与再利用国家重点实验室）攻读材料学博士学位。入选兰州理工大学优秀博士论文培育计划，获得国家重点实验室优秀博士生赴国（境）外留学项目资助。主要研究方向为金属基电池中金属阳极的失效机制和抑制失效研究。公开发表的代表性学术成果：
[1]Lei Zhao, Fen Ran*, Electrolyte-Philicity of Electrode Materials, Chemical Communications, 2023, 59, 6969-6986. 主题文章（Feature Article）、主编邀稿(Invited by Editor-in-chief)、封面文章（Front Cover）. (影响因子：6.065；中科院2区). https://doi.org/10.1039/D3CC00412K.
[2]Lei Zhao, Yuanyou Peng, Fen Ran*, Constructing Mutual-Philic Electrode/Non-Liquid Electrolyte Interfaces in Electrochemical Energy Storage Systems: Reasons, Progress, and Perspectives, Energy Storage Materials 2023, 58: 48-73. (影响因子：20.831；中科院1区). https://doi.org/10.1016/j.ensm.2023.03.009.
[3]Lei Zhao, Yuan Li, Meimei Yu, Yuanyou Peng, Fen Ran*, Electrolyte-Wettability Issues and Challenges of Electrode Materials in Electrochemical Energy Storage, Energy Conversion, and Beyond, Advanced Science 2023, 10(17): 2300283. (影响因子：17.521；中科院1区). http://dx.doi.org/10.1002/advs.202300283.
[4]Wenlin Zhang#, Lei Zhao#（共同一作）, Hui Li, Pantrangi Manasa, Fen Ran*, Hydrated halide clusters on electrode materials for aqueous supercapacitor. Journal of Power Sources 2021, 491: 229612. (影响因子：9.794；中科院2区). https://doi.org/10.1016/j.jpowsour.2021.229612.
[5] Qianqian Zhang,Lei Zhao, Hezhen Yang, Lingbin Kong, Fen Ran*, Alkali-Tolerant Polymeric Gel Electrolyte Membrane Based on Cross-linked Carboxylated Chitosan for Supercapacitors, Journal of Membrane Science 2021, 629: 119083. https://doi.org/10.1016/j.memsci.2021.119083.
[6]Lei Zhao, Yongtao Tan*, Fen Ran*, Rational Ratio of Quinoid Imine to Benzenoid Amine via In-Situ Doping with Gold Nanoparticles for Electrochemically Activation of Polyaniline, Journal of Materials Science: Materials in Electronics 2022, 33: 2138-2151. https://doi.org/10.1007/s10854-021-07421-0.
Abstract: In the past few decades, electrochemical energy storage systems, represented by alkali metal ion batteries and supercapacitors, have developed rapidly against the background of sustainable development. However, supercapacitors and alkali metal ion batteries, known for the high power density and high energy density, respectively, have struggled to meet the demand of high both power and energy densities energy storage devices. Therefore, integrating both energy storage mechanisms of supercapacitors and alkali metal ion batteries in the same system to attain device with comparatively high both power and energy densities has become the preferred approach for most researchers, and the representatives are assembling hybrid ion capacitors or introducing capacitive contribution into alkali metal ion batteries materials for fast-charging alkali metal ion batteries. For the former, many good quality publications have summarized and evaluated it, while the latter has not. In this review, we systematically summarize and insightfully discuss the phenomenon of introducing capacitive contribution into electrode materials of alkali metal ion batteries. Different methods of identifying capacitive and diffusive be[1]haviors are reviewed, and the origin of the capacitive contribution in the battery materials combining the charge storage mechanism are explained, the influences of electrode materials’ capacitive contribution on battery’s energy and power densities are discussed in detail. Finally, we propose a design idea of electrode materials for battery with high both power and energy densities based on accurately understanding the rational capacitive contribution.
何天启博士(Dr. Tianqi He)：2018年至今，在兰州理工大学材料科学与工程学院（有色金属先进加工与再利用国家重点实验室）攻读材料学博士学位（硕博连读）。获得博士生国家奖学金，入选兰州理工大学优秀博士论文培育计划。公开发表的代表性学术成果：
[1]Tianqi He, Xiaoya Kang, Fujuan Wang, Junlei Zhang, Tianyun Zhang, Fen Ran*, Capacitive Contribution Matters in Facilitating High Power Battery Materials Toward Fast-Charging Alkali Metal Ion Batteries, Materials Science & Engineering R-Reports 2023,154: 100737. (影响因子：33.667；中科院1区) https://doi.org/10.1016/j.mser.2023.100737.
[2]Tianqi He, Qiuping Zhao, Qianghong Wu, Junlei Zhang, Fen Ran*, Surfactant Induced Self-Assembly to Prepare Vanadium Nitride/N, S Co-doped Carbon as High-Capacitance Anode Materials. Chemical Communications 2021, 2021, 57, 10246-10249. (影响因子：6.065；中科院2区) https://doi.org/10.1039/d1cc04143f.
[3]Qianghong Wu#, Tianqi He# (共同一作), Yikai Zhang, Junlei Zhang, Zhijun Wang, Ying Liu, Lei Zhao, Youzhi Wu, Fen Ran*, Cyclic Stability of Supercapacitors: Materials, Energy Storage Mechanism, Test Methods, and Device, Journal of Materials Chemistry A 2021, 9, 24094-24147. 期刊邀请封面文章. (影响因子：14.511；中科院2区) https://doi.org/10.1039/d1ta06815f.
[4] Tianqi He, Xiaoya Kang, Fujuan Wang, Rui Wang, Lei Zhao, Yuanyou Peng, Fen Ran*, Designing Capacitive Contribution in Hard Carbon Materials for Balancing Energy and Power Under High Current Density for Sodium Ion Batteries, ACS Applied Energy Materials2023, 6(15): 8149-8157. (影响因子：6.4；中科院3区) https://doi.org/10.1021/acsaem.3c01291.
[5]Tianqi He, Mengyuan Tu, Junlei Zhang, Lingbin Kong, Fen Ran*, Nanopaticles of Iron Nitride Encapsulated in Nitrogen-Doped Carbon Bulk Derived from Polyaniline/Fe2O3 Blends and Its Electrochemical Performance. Particles & Particle Systems Characterization 2020, 37(7): 2000132. 期刊邀请封面文章. https://doi.org/10.1002/ppsc.202000132.
[6]Tianqi He, Wenlin Zhang, Pantrangi Manasa, Fen Ran*, Quantum Dots of Molybdenum Nitride Embedded in Continuously Distributed Polyaniline for Supercapacitor. Journal of Alloys and Compounds 2020, 812: 152138. ESI高被引论文. https://doi.org/10.1016/j.jallcom.2019.152138.
[7]Tianqi He, Zhen Wang, Xiaoming Li, Yongtao Tan, Ying Liu, Lingbin Kong, Long Kang, Chengmeng Chen, Fen Ran*, Intercalation structure of vanadium nitride nanoparticles growing on graphene surface toward high negative active material for supercapacitor utilization. Journal of Alloys and Compounds 2019, 781: 1054-1058. (Apr. 15 2019). ESI高被引论文. https://doi.org/10.1016/j.jallcom.2018.12.149.
