All-Electrochem-Active Graphite Electrode Enabled by Manipulating Li+ Activity of Inactive Components for High-Energy Batteries

The dataset contains the following six Figures and one Table: Figure 1. Schematic depicting a typical electrode (left) and the all-electrochem-active graphite electrode (right), with inset schemes showing transport of lithium ions in the TiO2−x@C conductive additives (top) and MXene binders (bottom). For detailed morphological characterization, please refer to the SEM images in Figure S1 in Supporting Information.pdf Figure 2. (a) Optical image, (b) SEM image, (c) TEM image, (d) XRD pattern, (e) FTIR spectrum, and (f) O 1s XPS spectrum of MXene. (g) CV of the MXene electrode at a scan rate of 0.2 mV s−1. (h) Cycling performance of the MXene electrode at 0.2C. (i) Voltage-capacity curves of MXene electrode at different current densities Figure 3. (a) SEM image, (b) TEM image, (c) STEM image, and corresponding elemental mappings of TiO2−x@C. (d) Electrical conductivity tests of TiO2−x@C and commercial carbon black SP. (e) XRD pattern and (f) O 1s XPS spectrum of TiO2−x@C. (g) CV of the TiO2−x@C electrode at a scan rate of 0.2 mV s−1. (h) Cycling performance of the TiO2−x@C electrode at 0.2C. (i) Voltage-capacity curves of the TiO2−x@C electrode at different current densities Figure 4. (a) CV of the AEA-G electrode during the first three cycles at a scan rate of 0.1 mV s−1. (b) Voltage-capacity curves of the AEA-G and PS-G electrodes in the first cycle. (c) Rate performance, (d) long-term cycling performance at 0.2C, (e) average CE, and (f) long-term cycling performance at 1C of the AEA-G and PS-G electrode. Mass loading of all electrodes is 1.2 mg cm−2. (g) Comparison of the electrochemical performance of the AEA-G electrode with graphite electrodes reported in the literature Figure 5. (a) EIS curves. (b) RSEI statistics and (c) Rct statistics of the AEA-G and PS-G electrodes in different cycles. (d) CVs obtained at different scanning rates. (e) Relationship between the peak current and scan rate of the AEA-G electrode. (f) Contribution ratios of the capacitive and diffusion-controlled processes at different scanning rates for the AEA-G and PS-G electrodes. (g) GITT curves of the AEA-G electrode. (h) Li+ diffusion coefficients for the AEA-G and PS-G electrodes during the delithiation process Figure 6. In situ XRD patterns of (a) AEA-G electrode and (b) PS-G electrode recorded during lithiation and delithiation processes. SEM image of (c) AEA-G electrode and (d) PS-G electrode after 100 cycles of charge and discharge. (e) Raman spectra of AEA-G electrode after 100 cycles of charge and discharge. (f) Raman spectra, (g) F 1s and (h) O 1s XPS spectrum of AEA-G electrode and PS-G electrode after 100 cycles of charge and discharge Table 1. Comparison of the Different Parameters of the AEA-G and PS-G Electrodes Funding: This work was supported by the following: European Union’s Horizon Europe Research and Innovation Program under grant agreement No. 101087143 (Electron Beam Emergent Additive Manufacturing (EBEAM) RE-FRESH Research Excellence for Region Sustainability and High-tech Industries (Project No. CZ.10.03.01/00/22 003/0000048) via an EU operational program National Natural Science Foundation of China (Grant No. 52071225) Norway Grants project No. 2019/34/H/ST8/00547 through the National Science Centre National Key R&D Program of China (2021YFB3800300) National Natural Science Foundation of China (Grant Nos. 22179143 and 22002176). Jiangsu Funding Program for Excellent Postdoctoral Talent.本数据集包含以下六幅图与一张表格： 图1 典型电极（左）与全电化学活性石墨电极（右）的结构示意图，内嵌示意图分别展示了TiO₂₋ₓ@C导电添加剂（上）与MXene粘结剂（下）中锂离子的传输过程。如需获取详细形貌表征结果，请参阅Supporting Information.pdf中的图S1的扫描电子显微镜（Scanning Electron Microscope, SEM）图像。 图2 (a) MXene的光学照片、(b) 扫描电子显微镜（Scanning Electron Microscope, SEM）图像、(c) 透射电子显微镜（Transmission Electron Microscope, TEM）图像、(d) X射线衍射（X-ray Diffraction, XRD）图谱、(e) 傅里叶变换红外光谱（Fourier Transform Infrared Spectroscopy, FTIR）谱图以及(f) O 1s X射线光电子能谱（X-ray Photoelectron Spectroscopy, XPS）谱图；(g) 扫描速率为0.2 mV·s⁻¹时MXene电极的循环伏安（Cyclic Voltammetry, CV）曲线；(h) 0.2C倍率下MXene电极的循环性能；(i) 不同电流密度下MXene电极的电压-容量曲线。 图3 (a) TiO₂₋ₓ@C的扫描电子显微镜（Scanning Electron Microscope, SEM）图像、(b) 透射电子显微镜（Transmission Electron Microscope, TEM）图像、(c) 扫描透射电子显微镜（Scanning Transmission Electron Microscope, STEM）图像及对应的元素分布图；(d) TiO₂₋ₓ@C与商用炭黑SP的电导率测试结果；(e) TiO₂₋ₓ@C的X射线衍射（X-ray Diffraction, XRD）图谱与(f) O 1s X射线光电子能谱（X-ray Photoelectron Spectroscopy, XPS）谱图；(g) 扫描速率为0.2 mV·s⁻¹时TiO₂₋ₓ@C电极的循环伏安（Cyclic Voltammetry, CV）曲线；(h) 0.2C倍率下TiO₂₋ₓ@C电极的循环性能；(i) 不同电流密度下TiO₂₋ₓ@C电极的电压-容量曲线。 图4 (a) 扫描速率为0.1 mV·s⁻¹时AEA-G电极前三个循环的循环伏安（Cyclic Voltammetry, CV）曲线；(b) 首圈循环中AEA-G与PS-G电极的电压-容量曲线；(c) 倍率性能、(d) 0.2C倍率下的长循环性能、(e) 平均库仑效率（Coulombic Efficiency, CE）以及(f) 1C倍率下的长循环性能：AEA-G与PS-G电极的活性物质负载量均为1.2 mg·cm⁻²；(g) AEA-G电极与文献报道的石墨电极电化学性能对比。 图5 (a) 电化学阻抗谱（Electrochemical Impedance Spectroscopy, EIS）曲线；(b) 不同循环圈数下AEA-G与PS-G电极的界面膜电阻（Solid Electrolyte Interphase Resistance, RSEI）统计值与(c) 电荷转移电阻（Charge Transfer Resistance, Rct）统计值；(d) 不同扫描速率下的循环伏安曲线；(e) AEA-G电极的峰电流与扫描速率的关系；(f) 不同扫描速率下AEA-G与PS-G电极的电容控制过程与扩散控制过程的贡献率；(g) AEA-G电极的恒电流间歇滴定技术（Galvanostatic Intermittent Titration Technique, GITT）曲线；(h) 脱锂过程中AEA-G与PS-G电极的锂离子扩散系数。 图6 (a) AEA-G电极与(b) PS-G电极在充放电过程中记录的原位X射线衍射（X-ray Diffraction, XRD）图谱；(c) 100次充放电循环后AEA-G电极与(d) PS-G电极的扫描电子显微镜（Scanning Electron Microscope, SEM）图像；(e) 100次充放电循环后AEA-G电极的拉曼光谱；(f) 拉曼光谱、(g) F 1s与(h) O 1s X射线光电子能谱（X-ray Photoelectron Spectroscopy, XPS）谱图：100次充放电循环后AEA-G与PS-G电极的对应测试结果。 表1 AEA-G与PS-G电极的不同参数对比 基金资助： 本研究得到以下项目资助： 欧盟地平线欧洲研究与创新计划，项目协议编号101087143，项目名称：电子束涌现增材制造（Electron Beam Emergent Additive Manufacturing, EBEAM）； 通过欧盟运营计划资助的区域可持续性与高科技产业研究卓越计划（RE-FRESH），项目编号：CZ.10.03.01/00/22 003/0000048； 国家自然科学基金，项目编号：52071225； 波兰国家科学中心牵头的挪威援助项目，项目编号：2019/34/H/ST8/00547； 中国国家重点研发计划，项目编号：2021YFB3800300； 国家自然科学基金，项目编号：22179143与22002176； 江苏省优秀博士后人才资助计划。