One-pot synthesis of high-capacity silicon-lithium anodes via on-copper growth of a semi-conducting, porous polymer

[This repository contains the source data for the manuscript <strong>"One-pot synthesis of high-capacity silicon-lithium anodes <em>via</em> on-copper growth of a semi-conducting, porous polymer"</strong>] Silicon-based anodes with lithium ions as charge carriers have the highest predicted charge density of 3579 mA h g^-1 (for Li₁₅Si₄) while being comparatively safe. Contemporary electrodes do not achieve these theoretical values largely because production paradigms remained unchanged since their inception and rely on the mixing of weakly coordinated, multiple components. In this paper, we present the one-pot synthesis of high-performance anodes that reach the theoretical capacity of the fully lithiated state of silicon. Here, a semi-conductive triazine-based graphdiyne polymer network is grown around silicon nanoparticles directly on the current collector, a copper sheet. The current collector (Cu) acts as the catalyst for the formation of a semi-conductive triazine-based graphdiyne polymer network that grows around the inorganic, active material (Si). In comparison to established electrode assemblies, this process (i) omits any steps related to curing, drying, and annealing, (ii) does away with binders and conductivity-enhancing additives that decrease volumetric and gravimetric capacity, and (iii) cancels out the detrimental effects on performance, chemical and physical stability of conventional, three-component anodes (Si, binder, carbon black). This is because, the porous, semi-conducting organic framework (i) adheres to the current collector on which it grows <em>via</em> cooperative van der Waals interactions, (ii) acts effectively as conductor for electrical charges and binder of silicon nanoparticles <em>via</em> conjugated, covalent bonds, and (iii) enables selective transport of mass and charge-carriers (electrolyte and Li-ions) through pores of defined size. As a result, the anode shows extraordinarily high capacity at the theoretical limit of fully lithiated silicon, excellent performances in terms of cycling (exceeding 70% capacity retention after 100 cycles), and high mechanical and thermal stability. These high-performance anodes pave the way for use in flexible, wearable electronics and in environmentally demanding applications.本仓库收录了论文**"基于铜基底原位生长半导体多孔聚合物一锅法制备高容量硅基锂阳极"**的源实验数据。以锂离子为电荷载体的硅基阳极（silicon-lithium anodes），其理论电荷密度最高可达3579 mA·h·g⁻¹（对应Li₁₅Si₄物相），且安全性相对优异。当前商用电极难以达到该理论性能指标，核心症结在于其生产范式自问世以来未发生本质变革，且依赖多组分弱配位混合工艺。本文报道了一种高性能阳极的一锅法（one-pot synthesis）合成策略，可实现硅完全锂化状态下的理论容量。该工艺将半导体三嗪基石墨炔聚合物网络直接生长于集流体（current collector，铜箔）表面的硅纳米颗粒周围。其中，集流体（Cu）可作为催化剂，促使无机活性材料（Si）周围形成半导体三嗪基石墨炔聚合物网络。与传统电极组装工艺相比，该制备流程具备三大核心优势：(i) 省去固化、干燥与退火等全部辅助工序；(ii) 无需使用会降低体积与重量比容量的粘结剂与导电增强添加剂；(iii) 消除了传统三组分阳极（硅、粘结剂、炭黑）对器件性能、化学与物理稳定性的负面影响。该多孔半导体有机骨架之所以具备上述优势，源于其三重特性：(i) 通过协同范德华作用力牢固附着于生长基底集流体；(ii) 凭借共轭共价键有效充当电荷传导介质与硅纳米颗粒的粘结剂；(iii) 通过孔径精准可控的多孔结构，实现电解质与锂离子等质量及电荷载体的选择性传输。最终，该阳极可在硅完全锂化的理论容量极限下展现出超高容量，循环性能优异（100次循环后容量保持率超过70%），同时具备出色的机械与热稳定性。这类高性能阳极为柔性可穿戴电子设备以及严苛环境应用场景开辟了可行路径。