用单次静态光谱预测锂电池SEI的动态红外变化,推动电化学AI发现。
From Static Spectra to Operando Infrared Dynamics: Physics Informed Flow Modeling and a Benchmark
- 基于物理约束设计双流框架,显式建模化学反应轨迹。
- 在7118样本数据集上,预测精度显著超越现有模型。
- 可泛化到未见电池体系,助力揭示SEI形成路径。
固态电解质界面(SEI)对锂离子电池性能至关重要,但原位红外(IR)光谱分析实验复杂且昂贵,限制了其在常规研究设施中的应用。为突破这一瓶颈,我们提出新任务:从单次静态光谱预测时间分辨的光谱“指纹”演化。为此,我们构建了首个大规模原位数据集OpIRSpec-7K,包含7,118个高质量样本,覆盖10种不同电池体系,并开发了评估基准OpIRBench。针对传统谱图、视频和序列模型在捕捉电压驱动化学动态与复杂组分方面的不足,我们提出端到端物理感知框架ABCC。该框架重构均值流,引入新型化学流以显式建模反应轨迹,采用双流解耦机制分离溶剂与SEI信号,并施加质量守恒与峰位移动等物理与谱图约束。ABCC显著优于最先进的静态、序列与生成基线模型,且能泛化至未见系统,支持可解释的下游SEI形成路径恢复,推动人工智能驱动的电化学发现。
原文摘要 · Abstract (English)
The Solid Electrolyte Interphase (SEI) is critical to the performance of lithium-ion batteries, yet its analysis via Operando Infrared (IR) spectroscopy remains experimentally complex and expensive, which limits its accessibility for standard research facilities. To overcome this bottleneck, we formulate a novel task, Operando IR Prediction, which aims to forecast the time-resolved evolution of spectral ``fingerprints'' from a single static spectrum. To facilitate this, we introduce OpIRSpec-7K, the first large-scale operando dataset comprising 7,118 high-quality samples across 10 distinct battery systems, alongside OpIRBench, a comprehensive evaluation benchmark with carefully designed protocols. Addressing the limitations of standard spectrum, video, and sequence models in capturing voltage-driven chemical dynamics and complex composition, we propose Aligned Bi-stream Chemical Constraint (ABCC), an end-to-end physics-aware framework. It reformulates MeanFlow and introduces a novel Chemical Flow to explicitly model reaction trajectories, employs a two-stream disentanglement mechanism for solvent-SEI separation, and enforces physics and spectrum constraints such as mass conservation and peak shifts. ABCC significantly outperforms state-of-the-art static, sequential, and generative baselines. ABCC even generalizes to unseen systems and enables interpretable downstream recovery of SEI formation pathways, supporting AI-driven electrochemical discovery.
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