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Publications
(# equal contribution; * corresponding)

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[1] Lei Liu, Jianhui Wang,* Overcoming Copper Substrate Thermodynamic Limitations in Anode-Free Lithium Pouch Cells via In Situ Seed Implantation, Nano Letters, 23 (2023), 10251–10258. [“36秒植晶”即可让437 Wh/kg无负极软包锂电池增寿一倍]

   

 

 

 

 

 

 

 

 

 

 

 

 

The application of in-situ seed implementation to generate uniform and densely-packed nano-sized lithium nuclei offers an effective solution to overcome the limitations imposed by the lithiophobic copper substrate in an anode-free lithium metal pouch cell, resulting in a doubling of the 437 Wh/kg battery's lifespan.

 

[2] Juner Chen,# Han Zhang,# Mingming Fang,# Changming Ke,# Shi Liu,* Jianhui Wang,* Design of Localized High-Concentration Electrolytes via Donor Number, ACS Energy Letters, 8 (2023), 1723-1734. [基于500多个样品研究提出局域高浓度电解液的DN设计原则,并开发-40 ~ +100 °C宽温廉价的局域高浓度电解液]

 

                                   Universal Design Principle for Localized High-Concentration Electrolytes

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Through a comprehensive investigation involving over 500 samples, we have identified the donor number of solvents, rather than dielectric constant or polarity, as a more reliable parameter for determining the solution structure. This finding can significantly enhance the design and exploration of new electrolytes. A low-cost electrolyte was formulated, enabling high-voltage (>4.6 V) and wide-temperature (−40–100 °C) operation of lithium batteries.

  

[3] Rui Lin,# Changming Ke,# Juner Chen, Shi Liu,* Jianhui Wang,* Asymmetric donor-acceptor molecule regulated core-shell-solvation electrolyte for high-voltage aqueous batteries, Joule 6 (2022) 399-417. 

[设计新型核壳溶液结构全阻燃水系电解液,在空气中组装高电压锂离子电池]

 

                                   Three Year's Perseverance Spells Success

                                          目Tech+ :找到关键“配方” 西湖大学水系电池研究取得重要进展

 

 

 

 

 

 

 

 

 

Asymmetric donor-acceptor molecules such as methylurea (MU) can regulate the hydrogen-bonding network of aqueous electrolyte to form a peculiar nanoscale core-shell-like solvation structure, which not only breaks the physical restriction of limited lithium salt solubility in water but also effectively suppresses hydrogen evolution at low potentials toward 0.5 V versus Li+/Li. This simple approach truly inherits the high safety of aqueous electrolytes and substantially expands the electrochemical stability window without compromising its cost-effective property.

 

[4] Rui Lin, Jiahao Chen, Changming Ke, Shi Liu, Jianhui Wang,* A dilute fluorine-free electrolyte design for high-voltage hybrid aqueous batteries, Journal of Energy Chemistry, 77 (2023), 180-190. [设计低浓度无氟高电压水系电解液,打造低成本、环保安全、高比能水系电池]

 

 

 

 

 

 

 

 

 

 

 

 

Fluorinated salts and/or high salt concentrations are usually necessary to produce protective films on the electrodes for high-voltage aqueous batteries, yet these approaches increase the cost, toxicity and reaction resistances of battery. To realize a dilute fluorine-free electrolyte, we found that the selection of appropriate ingredients that have both high stability and strong interactions with water is critical to widen the potential window of electrolyte over 3 V while suppressing parasitic reactions on the electrodes, which boosts the development of low-cost, environmentally-friendly, high-power and high-energy-density aqueous batteries.

 

 

[5] Yongzhen Jin, Yang Liu, Ruyan Wu, Jianhui Wang,* Local tensile strain boosts the electrocatalytic ammonia oxidation reaction, 60 (2024), 1104-1107. [Selected as 2023 Emerging Investigators Themed Issue;引入局域拉应力降低Ni(II)→Ni(III)转化电位,降低电催化氨氧化起始电位]

 

 

 

 

 

 

 

 

 

 

 

 

The introduction of local tensile strain in Ni(OH)2 nanosheets accelerates the Ni(OH)2-to-NiOOH transition and boosts the electrocatalytic ammonia oxidation reaction (EAOR), i.e., reducing the onset potential by 80mV, doubling both the current density and N2 faradaic efficiency, and enabling 1000 hours of operation at 160 mA cm-2.

 

 

[6] Yongzhen Jin, Xin Chen, Jianhui Wang,* From inert to active: a cocktail-like mediation of an Ag/Ni mixture for electrocatalytic ammonia oxidation reaction, Chemical Communications, 58 (2022), 10631-10634. [Invited as Electrochemical Energy Themed Issue;手工混合金属粉末激发电催化氨氧化活性,解耦吸附与电化学过程,鉴定活性中心]

 

 

 

 

 

 

 

 

 

 

 

 

 

 

We report a highly selective electrocatalytic ammonia oxidation reaction (EAOR) induced by handmilling inert powders of silver (NH3 adsorber) and nickel (OH - adsorber and active site). This cocktail-like mediation provides a good model for mechanistic understanding of the EAOR, benefiting the development of effective non-noble metal catalysts for the EAOR.

 

[7] Mingming Fang,# Juner Chen,# Boyang Chen, Jianhui Wang,* Salt-solvent synchro-constructed robust electrolyte-electrode interphase for high-voltage lithium metal batteries, Journal of Materials Chemistry A, 2022, DOI: 10.1039/D2TA02267B. [Selected as 2022 Emerging Investigators Themed Issue;设计低浓度"单一溶质/单一溶剂"高电压电解液,实现NCM622/Li锂金属电池在3~4.6V、-30~+60 °C条件下稳定工作]

 

 

A simple electrolyte formula of “single salt single solvent” — 1 M LiDFOB in ES — enables the stable operation of an NCM622|Li full cell (2.5 mA h cm−2, N/P = 4) under harsh conditions of high voltage (4.6 V) and wide temperature range (−30 to 60 °C).

 

[8] Jingjing Huang,# Zhe Chen,# Jinmeng Cai, Tao Wang,* Jianhui Wang,* Activating copper oxide for stable electrocatalytic ammonia oxidation reaction via in-situ introducing oxygen vacancies, Nano Research, 2022, doi:10.1007/s12274-022-4279-5 [通过原位引入氧空位来激活惰性的CuO,获得了迄今最稳定的电催化氧化氨催化剂]

 

 

In-situ electrochemically introducing oxygen vacancies (Vo) not only turns the inactive CuO into efficient electrocatalytic ammonia oxidation reaction (EAOR) catalyst but also achieves a high stability of over 400 h at a high current density of ~ 200 mA cm−2. The presence of Vo on the CuO surface induces a remarkable upshift of the d-band center of active Cu site closer to the Fermi level, which significantly stabilizes the reaction intermediates (*NHx) and efficiently oxidizes NH3 into N2.

 

[9] Jianhui Wang,# Qifeng Zheng,# Mingming Fang,# Seongjae Ko, Yuki Yamada, Atsuo Yamada,* Concentrated electrolytes widen the operating temperature range of lithium-ion batteries, Advanced Science 8 (2021) 2101646. [实现-20 ~ +100 °C宽温锂离子全电池,构想无热管理系统的动力电池]

 

 

 

 

 

 

Salt-concentrated electrolytes can overcome various challenges for lithium-ion full cells that operate in a wide temperature range from -20 to 100 °C. This achievement contributes to building a novel power battery pack that requires no thermal management system and deliveries greatly enhanced systematic energy densities in both gravimetry and volumetry.

 

[10] Yuki Yamada,# Jianhui Wang,# Seongjae Ko, Eriko Watanabe, Atsuo Yamada,* Advances and issues in developing salt-concentrated battery electrolytes, Nature Energy 4 (2019) 269-280. 

  

 

[11] Jianhui Wang, Yuki Yamada, Keitaro Sodeyama, Eriko Watanabe, Koji Takada, Yoshitaka Tateyama, Atsuo Yamada*, Fire-extinguishing organic electrolytes for safe batteries, Nature Energy 3 (2018), 22-29.  [设计灭火有机电解液,实现安全长寿锂/钠离子电池]

 

  • 日本経済新聞、読売新聞

       JFS: Japanese Researchers Develop Flame-Retardant Electrolyte for Safer Batteries

       MEXT Element Strategy Initiative: Fire-Extinguishing Organic Electrolytes for Secondary Batteries

       化学者のつぶやき -Chem-Station-: リチウムイオンに係る消火剤電解液のはなし

       香港创新科技署:Battery with built-in "fire extinguisher"

 

 

 

 

 

 

 

 

 

 

 

Severe safety concerns are impeding the large-scale employment of lithium/sodium batteries. Conventional electrolytes are highly flammable and volatile, which may cause catastrophic fires or explosions. Efforts to introduce flame-retardant solvents into the electrolytes have generally resulted in compromised battery performance because those solvents do not suitably passivate carbonaceous anodes. Here we report a salt-concentrated electrolyte design to resolve this dilemma, achieving long-term cycling Li-, Na-ion batteries with better safety.

[12] Jianhui Wang, Yuki Yamada, Keitaro Sodeyama, Ching Hua Chiang, Yoshitaka Tateyama, Atsuo Yamada*, Superconcentrated electrolytes for a high-voltage lithium-ion Battery, Nature Communications 7 (2016), 12032. [设计首例“单一溶质单一溶剂”的高电压锂离子电解液,实现5V级电池]

 

                                          中国科学家在新高压锂电池技术上取得突破

 

 

 

 

 

 

 

 

Electrode degradation due to metal-ion dissolution in conventional electrolyte hampers the performance of 5 V-class Li-ion batteries. Here, we report a Simple mixing of a lithium salt and a solvent at super-high concentration leads to the formation of a three-dimensional network of solution structure. Without any additives, this new class of superconcentrated electrolytes overcome the long-standing challenge of metal ion dissolution at high voltages, and thus, realize a stable and high-rate 5 V-class LiNi0.5Mn1.5O4 | graphite battery.

 

[13] Jianhui Wang, Tao Liu, GuotaoWu, Wen Li, Yongfeng Liu, C. Moyses Araujo, Ralph H. Scheicher, Andres Blomqvist, Rajeev Ahuja, Zhitao Xiong, Ping Yang, Mingxia Gao, Hongge Pan, Ping Chen*, Ein Kalium-modifiziertes Mg(NH2)2-2LiH-System für die Wasserstoffspeicherung, Angewandte Chemie, 121 (2009), 5942-5946; Potassium-Modified Mg(NH2)2/2LiH System for Hydrogen Storage, Angewandte Chemie-International Edition, 48 (2009), 5828-5832. [首次研发了一种高效的非过渡金属储氢催化剂──钾,在107 °C附近可逆吸放氢~5wt%]

 

 

 

 

 

 

Using KH as an additive to Mg(NH2)2/LiH drastically improves hydrogen desorption, which begins at ca. 80 °C. Circa 5 wt% of hydrogen can be reversibly desorbed and absorbed at about 107 °C. The presence of potassium in the reacting system weakens the amide N—H and imide Li—N bonds, leading to enhanced reaction kinetics.

 

 

[14] Jianhui Wang, Ping Chen*, Hongge Pan, Zhitao Xiong, Mingxia Gao, Guotao Wu, Chu Liang, Cao Li, Jieru Wang, Solid-solid heterogeneous catalysis: The role of potassium in promoting the dehydrogenation of the Mg(NH2)2/2LiH composite, ChemSusChem, 6 (2013), 2181-2189. [揭示了钾的催化放氢机制,不同于常规过渡金属催化机理,为设计高效储氢催化剂提供了一种新思路]

 

 

 

Potassium is in the loop: The introduction of potassium to the Mg(NH2)2/2 LiH composite evolves intermediates of K2Mg(NH2)4, Li3K(NH2)4, and KH, which circularly transform between each other to create a more energy-favorable pathway for dehydrogenation, and thus contributes to the overall kinetic enhancement.

                                                                                                                                   

[15] Jianhui Wang*, Haiwen Li*, Ping Chen*, Amides and borohydrides for high-capacity solid-state hydrogen storage — materials design and kinetic improvements, MRS Bulletin, 38 (2013), 480-487.  

 

 

[16] Jianhui Wang, Jianjiang Hu, Yongfeng Liu, Zhitao Xiong, Guotao Wu, Hongge Pan, Ping Chen*, Effects of triphenyl phosphate on the hydrogen storage performance of the Mg(NH2)2-2LiH system, Journal of Materials Chemistry, 19 (2009), 2141-2146. [基于材料固态熵变化,构想了一种调变储氢材料热力学性能的新途径]

 

 

 

 

 

With the introduction of a small amount of triphenyl phosphate (TPP), Mg(NH2)2 keeps amorphous state during hydrogen sorption operation. Though the TPP-doped sample shows a faster reaction kinetics, the systematic equilibrium hydrogen pressure decreases as compared to the crystalline sample, which is likely due to the decrease of entropy change of Mg(NH2)2 in the system.

 

[17] Yatao Liu, Linhan Xu, Yongquan Yu, Mengxue He, Han Zhang, Yanqun Tang, Feng Xiong, Song Gao, Aijun Li, Jianhui Wang, ShenZhen Xu, Doron Aurbach, Ruqiang Zou, Quanquan Pang, Stabilized Li-S batteries with anti-solvent-tamed quasi-solid-state reaction, Joule, 7 (2023), 2074-2091.

 

[18] Yangfan Lin,# Juner Chen,# Han Zhang, Jianhui Wang,* In-situ Construction of High-Mechanical-Strength and Fast-Ion-Conductivity Interphase for Anode-free Li Battery, Journal of Energy Chemistry 80 (2023), 207-214.

[19] Jingjing Huang, Jinmeng Cai, Jianhui Wang,* Nanostructured Wire-in-Plate Electrocatalyst for High-Durability Production of Hydrogen and Nitrogen from Alkaline Ammonia Solution, ACS Applied Energy Materials 3 (2020) 4108-4113.

[20] Koji Takada, Yuki Yamada, Eriko Watanabe, Jianhui Wang, Keitaro Sodeyama, Yoshitaka Tateyama, Kazuhisa Hirata, Takeo Kawase, and Atsuo Yamada*, Unusual passivation ability of superconcentrated electrolytes toward hard carbon negative electrode in sodium-ion batteries, ACS Applied Materials & Interfaces, 9 (2017), 33802-33809.

[21] Yuki Yamada, Ching Hua Chiang, Keitaro Sodeyama, Jianhui Wang, Yoshitaka Tateyama, Atsuo Yamada*, Corrosion Prevention Mechanism of Aluminum Metal in Superconcentrated Electrolytes, ChemElectroChem, 2 (2015), 1687-1694.

[22] Huai-Jun Lin*, Hai-Wen Li, Biswajit Paik, Jianhui Wang and Etsuo Akiba, Improvement of hydrogen storage property of three-component Mg(NH2)2-LiNH2-LiH compositions by additives, Dalton Transactions, 45 (2016), 15374-15381.              

[23] Biswajit Paik, Hai-Wen Li*, Jianhui Wang, Etsuo Akiba, A Li-Mg-N-H composite as H2 storage material: a case study with Mg(NH2)2-4LiH-LiNH2, Chemical Communication, 51 (2015), 10018-10021.                                                          

[24] Hujun Cao, Jianhui Wang, Yongshen Chua, Han Wang, Guotao Wu, Zhitao Xiong, Jieshan Qiu, Ping Chen*, NH3 Mediated or Ion Migration Reaction: The Case Study on Halide-Amide System, Journal of Physical Chemistry C, 118 (2014), 2344-2349.

[25] Hujun Cao, Yao Zhang, Jianhui Wang, Zhitao Xiong, Guotao Wu, Jieshan Qiu, Ping Chen*, Effects of Al-based additives on the hydrogen storage performance of the Mg(NH2)2-2LiH system, Dalton Transactions, 42 (2013), 5524-5531.                  

             

[26] Hujun Cao, Yao Zhang, Jianhui Wang, Zhitao Xiong, Guotao Wu, Ping Chen*, Materials design and modification on amide-based composites for hydrogen storage, Progress in Natural Science: Materials International, 22 (2012), 550-560.

[27] Jianhui Wang, Guotao Wu, Yongshen Chua, Jianping Guo, Zhitao Xiong, Yao Zhang, Mingxia Gao, Hongge Pan, Ping Chen*, Hydrogen sorption from the Mg(NH2)2-KH system and synthesis of an amide-imide complex of KMg(NH)(NH2), ChemSusChem, 4 (2011), 1622-1628.

[28] Yanjing Yang, Mingxia Gao*, Yongfeng Liu, Jianhui Wang, Jian Gu, Hongge Pan, Zhengxiao Guo, Multi-hydride systems with enhanced hydrogen storage properties derived from Mg(BH4)2 and LiAlH4, International Journal of Hydrogen Energy, 37 (2012), 10733-10742.

[29] Yongfeng Liu, Kai Zhong, Mingxia Gao, Jianhui Wang, Hongge Pan*, Qidong Wang, Hydrogen storage in a LiNH2-MgH2 (1:1) system, Chemistry of Materials, 20 (2008), 3521-3527.

[30] Renbo Lin, Yongfeng Liu, Mingxia Gao, Jianhui Wang, Hongwei Ge, Hongge Pan*, Investigation on performances of the novel ammonia-based hydrogen storage material CaCl2, Journal of Inorganic Materials, 23 (2008), 1059-1063.

[31] Kai Zhong, Yongfeng Liu, Mingxia Gao, Jianhui Wang, He Miao, Hongge Pan*, Electrochemical kinetic performance of V-Ti-based hydrogen storage alloy electrode with different particle sizes, International Journal of Hydrogen Energy, 33 (2008), 149-155.

[32] He Miao, Mingxia Gao, Yongfeng Liu, Yan Lin, Jianhui Wang, Hongge Pan*, Microstructure and electrochemical properties of Ti-V-based multiphase hydrogen storage electrode alloys Ti0.8Zr0.2V2.7Mn0.5Cr0.8-xNi1.25Fex (x=0.0-0.8), International Journal of Hydrogen Energy, 32 (2007), 3947-3953.

[33] He Miao, Mingxia Gao, Yongfeng Liu, Yan Lin, Jianhui Wang, Hongge Pan*, Effects of Y substitution for Ti on the microstructure and electrochemical properties of Ti-V-Fe-based hydrogen storage alloys, Journal of the Electrochemical Society, 154(2007), A1010-A1014.                                      

                       

[34] Jianhui Wang, Hongge Pan*, Rui Li, Kai Zhong, Mingxia Gao, The effect of particle size on the electrode performance of Ti-V-based hydrogen storage alloys, International Journal of Hydrogen Energy, 32 (2007), 3381-3386.

[35] Jianhui Wang, Kai Zhong, Hui Ding, Rui Li, Mingxia Gao, Hongge Pan*, Structure and electrochemical properties of La-Mg-Ni system hydrogen storage alloys with different Co contents, Transactions of Nonferrous Metals Society of China, 15 (2005), 1351-1355.

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