电化学催化

电化学催化反应是实现电能和化学能相互转换的重要途径,是不少未来新能源技术的核心关键。我们课题组目前致力于CO2还原H2氧化、O2还原制H2O2关键反应的纳米电催化材料研究,通过设计和调控材料的组成、结构与表界面来提升反应的电催化活性、选择性和稳定性。在前期的工作中,我们课题组在CO2还原制备CO和甲酸、碱性体系下氢氧化等方面的研究取得了多项重要的研究成果,率先发展了一系列高效电化学催化材料,包括:大环过渡金属分子催化剂杂原子掺杂的碳材料用于实现CO的高选择性生成;若干新型的二维铋烯和钯基催化剂用于CO2还原制备甲酸盐;双功能的Ni3NNiMo合金用于高效的碱性氢氧化/析氢反应等。基于前期的研究基础,我们现阶段的工作集中在CO2/CO还原制备多碳(C2+)产物的研究、多级协同催化体系的构建以及新型非贵金属基氢氧化催化剂的开发等领域。此外,为了推进碳资源转化技术的发展,我们课题组以技术应用为导向,在电催化反应装置的研制和面向大规模应用的工艺流程开发等方面也进行了一定尝试。

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

 

代表性工作:

1. Lin Jia#, Mingzi Sun#, Jie Xu#, Xuan Zhao, Rui Zhou, Binbin Pan, Lu Wang, Na Han, Bolong Huang* and Yanguang Li* Phase-Dependent Electrocatalytic CO2 Reduction on Pd3Bi Nanocrystals. Angew. Chem. Int. Ed. 2021, 60, 21741-21745.  

2. Yang Huang#, Xinnan Mao#, Guotao Yuan, Duo Zhang, Binbin Pan, Jun Deng, Yunru Shi, Na Han, Chaoran Li, Liang Zhang, Lu Wang*, Lin He*, Youyong Li and Yanguang Li* Size-Dependent Selectivity of Electrochemical CO2 Reduction on Converted In2O3 Nanocrystals. Angew. Chem. Int. Ed. 20216015844-15848.

3. Miao Wang#, Hao Yang#, Jinan Shi, Yufeng Chen, Yuan Zhou, Liguang Wang, Sijia Di, Xuan Zhao, Jun Zhong, Tao Cheng, Wu Zhou, and Yanguang Li* Alloying Nickel with Molybdenum Significantly Accelerates Bifunctional Hydrogen Electrocatalysis in Alkaline Solution. Angew. Chem. Int. Ed. 202160, 5771-5777.

4. Jia Fan, Xuan Zhao, Xinnan Mao, Jie Xu, Na Han, Hao Yang, Binbin Pan, Yongshen Li, Lu Wang, Yanguang Li* Large-Area Vertically-Aligned Bismuthene Nanosheet Arrays from Galvanic Replacement Reaction for Efficient Electrochemical CO2 Conversion. Adv. Mater. 202133, 2100910.

5. Na Han#, Mingzi Sun#, Yuan Zhou, Jie Xu, Chen Cheng, Rui Zhou, Liang Zhang, Jun Luo, Bolong Huang* and Yanguang Li* Alloyed Palladium-Silver Nanowires Stabilizing Carbon Dioxide Reduction to Formate. Adv. Mater. 202133, 2005821

6. Yuan Zhou#, Rui Zhou#, Xiaorong Zhu, Na Han, Bin Song, Tongchao Liu, Guangzhi Hu, Yafei Li, Jun Lu* and Yanguang Li* Mesoporous PdAg Nanospheres for Stable Electrochemical CO2 Reduction to Formate. Adv. Mater2020, 32, 2000992.

7. Xuan Zhao#, Yu Wang#, Yunli Da#, Xinxia Wang, Tingting Wang, Mingquan Xu, Xiaoyun He, Wu Zhou*, Yafei Li*, Jonathan N. Coleman and Yanguang Li* Selective Electrochemical Production of Hydrogen Peroxide at Zigzag Edges of Exfoliated Molybdenum Telluride Nanoflakes. Natl. Sci. Rev. 20207, 1360-1366.

8. Tingting Wang#, Miao Wang#, Hao Yang#, Mingquan Xu, Chuandong Zuo, Kun Feng, Miao Xie, Jun Deng, Jun Zhong, Wu Zhou, Tao Cheng* and Yanguang Li* Weakening Hydrogen Adsorption on Nickel via Interstitial Nitrogen Doping Promotes Bifunctional Hydrogen Electrocatalysis in Alkaline Solution. Energy Environ. Sci. 2019643522-3529.

9. Qiufang Gong#, Pan Ding#, Mingquan Xu#Xiaorong Zhu#, Maoyu Wang#, Jun Deng, Qing Ma, Na Han, Yong Zhu, Jun Lu, Zhenxing Feng*, Yafei Li*, Wu Zhou* and Yanguang Li* Structural Defects on Converted Bismuth Oxide Nanotubes Enable Highly Active Electrocatalysis of Carbon Dioxide reduction. Nature Commun. 201910, 2807.

10. Na Han#, Yu Wang#, Hui Yang, Jun Deng, Jinghua Wu, Yafei Li* and Yanguang Li* Ultrathin Bismuth Nanosheets from In-Situ Topotactic Transformation for Selective Electrocatalytic CO2 Reduction to Formate. Nature Commun. 20189, 1320.

11. Na Han, Lu Ma, Jianguo Wen, Jing Li, Hechuang Zheng, Kaiqi Nie, Xinxia Wang, Feipeng Zhao, Yafei Li*, Jian Fan, Jun Zhong, Tianping Wu, Dean J. Miller, Jun Lu*, Shuit-Tong Lee and Yanguang Li*, Supported Cobalt Polyphthalocyanine for High-Performance Electrocataltyic CO2ReductionChem 20173652-664

 

新型电池

化学电池是通过电能和化学能相互转换实现能量有效储存的装置。以锂离子电池为代表的传统电池技术因其成本和安全性问题,其发展已进入瓶颈期。针对上述挑战,我们课题组尝试通过对正负极电极材料的合理构筑、加工和优化,希望开发高安全性、高循环稳定性、高能量密度和低成本的新型电池体系,包括碱金属离子电池金属-硫电池、金属-空气电池。课题组代表性的工作包括:发展了无定型MoS3作为高性能钠离子电池材料和锂/钠/钾-硫电池“类硫”正极材料,获得了良好的电极容量和循环稳定性;报道了泡沫铜集流体化学固硫作用,发展了WxC、Mo2C材料化学固硫和电催化多硫化物转化作用,缓解了金属-硫电池中的“穿梭效应”问题;设计了简单的碱金属负极保护方法,使用碳纸或硅抑制了锂/钠/钾枝晶的生长。目前,我们的研究主要集中在碱金属离子电池和多价离子电池的无机/有机纳米电极材料设计上,研究材料结构与电化学性能之间的构效关系,希望发现一些新的规律和现象。

 

 

代表性工作:

1. Yunling Wu#, Xinnan Mao#, Mochun Zhang, Xuan Zhao, Renjie Xue, Sijia Di, Wei Huang, Lu Wang*, Youyong Li and Yanguang Li* Two-Dimensional Molecular Sheets of Hydrogen-Bonded Organic Frameworks for Ultrastable Sodium-Ion Storage. Adv. Mater. 202133, 2106079.

2. Hualin Ye* and Yanguang Li* Review on Multivalent Rechargeable Metal-Organic Batteries. Energy Fuels 202135, 7624-7636.

3. Yulei Sui, Jian Zhou, Xiaowei Wang, Ling Wu*Shengkui Zhong* and Yanguang Li* Recent Advances in Black-Phosphorus-Based Materials for Electrochemical Energy Storage, Mater. Today 202142, 117-136. 

4. Hualin Ye, Matthew Li, Tongchao Liu, Yanguang Li* and Jun Lu* Activating Li2S as the Lithium-Containing Cathode in Lithium-Sulfur Batteries. ACS Energy Lett. 20205, 2234-2245. 

5. Tianhui Xu, Peng Gao, Peirong Li, Kai Xia, Na Han, Jun Deng, Yanguang Li* and Jun Lu* Fast-Charging and Ultrahigh-Capacity Lithium Metal Anode Enabled by Surface Alloying. Adv. Energy Mater. 2020, 10, 1902343.

6. Yunling Wu#, Xiaorong Zhu#, Peirong Li, Tao Zhang, Mattew Li, Jun Deng, Yang Huang, Pan Ding, Sixia Wang, Rui Zhang, Jun Lu*, Guang Lu*, Yafei Li* and Yanguang Li* Ultradispersed WxC Nanoparticles Enable Fast Polysulfide Interconversion for High-Performance Li-S Batteries. Nano Energy 201959, 636-643.

7. Peirong Li, Tianhui Xu, Pan Ding, Jun Deng, Chenyang Zha, Yunling Wu, Yeyun Wang and Yanguang Li* Highly Reversible Na and K Metal Anodes by Carbon Paper Protection. Energy Storage Mater. 201815, 8-13.

8. Junhua Zhou#, Lu Wang#, Mingye Yang, Jinghua Wu, Fengjiao Chen, Wenjing Huang, Na Han, Hualin Ye, Feipeng Zhao, Youyong Li and Yanguang Li* Hierarchical VS2 Nanosheet Assembies: A Universal Host Material for the Reversible Storage of Alkali Metal Ions. Adv. Mater. 201729, 1702061.

9. Hualin Ye#, Lu Ma#, Yu Zhou, Lu Wang, Na Han, Feipeng Zhao, Jun Deng, Tianpin Wu, Yanguang Li*, Jun Lu* Amorphous MoS3 as the Sulfur-Equivalent Cathode Material for Room-Temperature Li-S and Na-S Batteries, Proc. Natl. Acad. Sci. 2017114, 13091-13096.

 

光催化

   人工光合成通过模拟自然界植物光合作用,利用太阳能将CO2H2O转化为清洁燃料,为能源的生产提供了一条绿色、可持续的途径。实现这一目标的关键是开发高效的半导体光催化材料。本课题组最近以有机聚合物半导体材料为主要研究对象,探索它们在光催化CO2还原H2O裂解以及生物质转化等领域的应用。借助有机材料灵活的分子设计,从分子层面对有机半导体的光电特性、表面性质进行优化调控,提高光催化反应活性和产物选择性,并结合多种表征手段揭示材料结构和催化性能之间的构效关系。在最近的研究中,我们利用逐步聚合物方法,构筑了共价键联的共价三嗪聚合物(CTFs)异质结,有效抑制光生电荷的复合,极大提升光催化析氢的活性;利用D-A型聚合物半导体作为光催化剂在可见光照射下直接活化水溶液中H+,实现对不饱和双键的氢化还原,获得具有高附加值的有机化学品。在现阶段,我们的研究主要集中在结晶的二维共价有机框架材料(2D-COFs)的合成及其光催化应用研究。另外,我们也积极探索新型有机-无机杂化的光催化体系构筑及其在能源光催化方面的应用。

 

 

代表性工作:

1. Wei Huang, Wei Luo, Yanguang Li* Two-Dimensional Semiconducting Covalent Organic Frameworks for Photocatalytic Solar Fuel Production. Mater. Today 2020, in press. DOI: 10.1016/j.mattod.2020.07.003

2. Yongpan Hu#, Wei Huang#, Hongshuai Wang, Qing He, Yuan Zhou, Ping Yang, Youyong Li and Yanguang Li* Metal-Free Photocatalytic Hydrogenation Using Covalent Triazine Polymers. Angew. Chem. Int. Ed. 2020, 59, 14378-14382.

3. Wei Huang, Qing He, Yongpan Hu and Yanguang Li* Molecular Heterostructures of Covalent Triazine Frameworks for Highly Enhanced Photocatalytic Hydrogen Production. Angew. Chem. Int. Ed. 2019, 58, 8676-8680.