Assembly of N- and P-functionalized carbon nanostructures derived from precursor-defined ternary copolymers for high-capacity lithium-ion batteries

doi:10.1016/j.cjche.2022.01.032

Chinese Journal of Chemical Engineering ›› 2023, Vol. 53 ›› Issue (1): 280-288.DOI: 10.1016/j.cjche.2022.01.032

Assembly of N- and P-functionalized carbon nanostructures derived from precursor-defined ternary copolymers for high-capacity lithium-ion batteries

Luyao Guo¹, Mengru Wang¹, Ronghe Lin¹, Jiaxin Ma^2,3, Shuanghao Zheng^2,5, Xiaoling Mou¹, Jun Zhang⁴, Zhong-Shuai Wu^2,5, Yunjie Ding^1,2,5

1. Hangzhou Institute of Advanced Studies, Zhejiang Normal University, Hangzhou 311231, China;
2. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;
3. University of Chinese Academy of Sciences, Yuquan Road 19A, Shijingshan District, Beijing 100049, China;
4. College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, China;
5. Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, China

Received:2021-10-15 Revised:2022-01-05 Online:2023-04-08 Published:2023-01-28
Contact: Ronghe Lin,E-mail:catalysis.lin@zjnu.edu.cn;Jun Zhang,E-mail:jzhang2017@suda.edu.cn;Yunjie Ding,E-mail:dyj@dicp.ac.cn
Supported by:
We thank the financial support from Zhejiang Normal University (YS304320035, YS304320036), the National Key Research and Development Program of China (2016YFB0100100, 2016YFA0200200), the National Natural Science Foundation of China (51872283, 22075279, 21805273, 22005297, 22005298), the Liaoning Revitalization Talents Program (XLYC1807153), the Funds for Local Science and Technology Development by the Central Government of Liaoning Province (2021JH6/10500112), Dalian Innovation Support Plan for High Level Talents (2019RT09), Dalian National Laboratory For Clean Energy (DNL), CAS, DNL Cooperation Fund, CAS (DNL201912, DNL201915), and DICP (DICP ZZBS201708, DICP ZZBS201802, DICP I2020032).

Assembly of N- and P-functionalized carbon nanostructures derived from precursor-defined ternary copolymers for high-capacity lithium-ion batteries

Luyao Guo¹, Mengru Wang¹, Ronghe Lin¹, Jiaxin Ma^2,3, Shuanghao Zheng^2,5, Xiaoling Mou¹, Jun Zhang⁴, Zhong-Shuai Wu^2,5, Yunjie Ding^1,2,5

1. Hangzhou Institute of Advanced Studies, Zhejiang Normal University, Hangzhou 311231, China;
2. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;
3. University of Chinese Academy of Sciences, Yuquan Road 19A, Shijingshan District, Beijing 100049, China;
4. College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, China;
5. Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian 116023, China

通讯作者: Ronghe Lin,E-mail:catalysis.lin@zjnu.edu.cn;Jun Zhang,E-mail:jzhang2017@suda.edu.cn;Yunjie Ding,E-mail:dyj@dicp.ac.cn
基金资助:
We thank the financial support from Zhejiang Normal University (YS304320035, YS304320036), the National Key Research and Development Program of China (2016YFB0100100, 2016YFA0200200), the National Natural Science Foundation of China (51872283, 22075279, 21805273, 22005297, 22005298), the Liaoning Revitalization Talents Program (XLYC1807153), the Funds for Local Science and Technology Development by the Central Government of Liaoning Province (2021JH6/10500112), Dalian Innovation Support Plan for High Level Talents (2019RT09), Dalian National Laboratory For Clean Energy (DNL), CAS, DNL Cooperation Fund, CAS (DNL201912, DNL201915), and DICP (DICP ZZBS201708, DICP ZZBS201802, DICP I2020032).

Abstract

Abstract: Synthesis of new carbon nanostructures with tunable properties is vital for precisely regulating electrochemical performance in the wide applications. Herein, we report a novel approach for the oxidative polymerization of N- and P-bearing copolymers from the self-assembly of three different monomers (aniline, pyrrole, and phytic acid), and further prepare the respective carbon nanostructures with relatively consistent N dopant (6.2%–8.0%, atom) and varying P concentrations (0.4%–2.8%, atom) via controllable pyrolysis. The impacts of phytic acid addition on the compositional, structural, and morphological evolution of the copolymers and the resulting nanocarbons are well studied through a spectrum of characterizations including N₂ sorption, Fourier transform infrared spectroscopy, gel permeation chromatograph, scanning/transmission electron microscopy, and X-ray photoelectron spectroscopy. Gradual fragmentation of the nanosphere structures is evidenced with increasing addition of phytic acid, leading to different nanostructures from hollow nanospheres to 3D aggregates. Nanocarbons decorated with N and P dopants from pyrolysis are further utilized as anode materials in lithium-ion batteries, demonstrating enhanced electrochemical performance, i.e., a reversible capacity of 380 mA·h·g^-1 at 2 A·g^-1 for NPC-0.5 during 200 cycles. The superior performance originates from the balanced porosity, and appropriate concentrations of P and pyrrolic N, thus pointing the direction for designing high-performance anode materials.

Key words: Carbon nanospheres, Doping, Lithium-ion batteries, Polymers, Porosity

摘要： Synthesis of new carbon nanostructures with tunable properties is vital for precisely regulating electrochemical performance in the wide applications. Herein, we report a novel approach for the oxidative polymerization of N- and P-bearing copolymers from the self-assembly of three different monomers (aniline, pyrrole, and phytic acid), and further prepare the respective carbon nanostructures with relatively consistent N dopant (6.2%–8.0%, atom) and varying P concentrations (0.4%–2.8%, atom) via controllable pyrolysis. The impacts of phytic acid addition on the compositional, structural, and morphological evolution of the copolymers and the resulting nanocarbons are well studied through a spectrum of characterizations including N₂ sorption, Fourier transform infrared spectroscopy, gel permeation chromatograph, scanning/transmission electron microscopy, and X-ray photoelectron spectroscopy. Gradual fragmentation of the nanosphere structures is evidenced with increasing addition of phytic acid, leading to different nanostructures from hollow nanospheres to 3D aggregates. Nanocarbons decorated with N and P dopants from pyrolysis are further utilized as anode materials in lithium-ion batteries, demonstrating enhanced electrochemical performance, i.e., a reversible capacity of 380 mA·h·g^-1 at 2 A·g^-1 for NPC-0.5 during 200 cycles. The superior performance originates from the balanced porosity, and appropriate concentrations of P and pyrrolic N, thus pointing the direction for designing high-performance anode materials.

关键词: Carbon nanospheres, Doping, Lithium-ion batteries, Polymers, Porosity

Luyao Guo, Mengru Wang, Ronghe Lin, Jiaxin Ma, Shuanghao Zheng, Xiaoling Mou, Jun Zhang, Zhong-Shuai Wu, Yunjie Ding. Assembly of N- and P-functionalized carbon nanostructures derived from precursor-defined ternary copolymers for high-capacity lithium-ion batteries[J]. Chinese Journal of Chemical Engineering, 2023, 53(1): 280-288.

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Assembly of N- and P-functionalized carbon nanostructures derived from precursor-defined ternary copolymers for high-capacity lithium-ion batteries

Assembly of N- and P-functionalized carbon nanostructures derived from precursor-defined ternary copolymers for high-capacity lithium-ion batteries

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