arXiv:2608.11283cond-mat.mtrl-scics.AI2026-08

用化学语言描述晶体结构,让大模型可解释地验证金属有机框架合理性。

Chemically Meaningful Textualization Enables Explainable Validation of Metal-Organic Frameworks by Large Language Models

  • 将晶格信息转化为化学语义文本,使大模型理解局部配位与连接关系。
  • 在识别不合理MOF上表现接近图模型,准确率超90%且能定位错误类型。
  • 生成诊断理由,适合材料数据库清洗与新手科研人员学习使用。

计算可用的金属有机框架(MOF)数据库对高通量筛选至关重要,但许多报道的晶体结构存在化学不合理或无序问题,影响模拟精度。现有验证方法依赖启发式规则、需授权许可或可解释性差。本文表明,当晶格信息被转化为化学语义文本后,大语言模型(LLMs)可作为可解释的MOF结构验证工具。通过对比九种描述符,发现成功验证不取决于信息量多少,而在于局部配位、框架连通性与化学背景是否形成语言可学习表示。使用专有描述符(mof2text)微调的LLM,在识别不合理MOF上表现与图模型相当(准确率>90%)。更重要的是,该模型不仅能输出分类结果,还能生成诊断依据,指出异常键合、连接性及电荷状态等问题,并预测错误类别。本研究确立了化学感知文本化是使大模型从通用文本模型转变为实用可解释的MOF数据库净化工具的关键步骤。

原文摘要 · Abstract (English)

Computation-ready metal-organic framework (MOF) databases are essential for high-throughput screening, yet many reported crystal structures remain chemically unreasonable or disordered, compromising simulation fidelity. Existing validation approaches can identify non-computation-ready structures, but they often rely on heuristic rules, license requirement, or offer limited interpretability. Here, we show that large language models (LLMs) can serve as interpretable validators of MOF structures when crystallographic information is transformed into chemically meaningful text. By benchmarking nine descriptors, we find that successful LLM-based validation depends not on the amount of structural information alone, but on whether local coordination, framework connectivity, and chemical context are organized into a linguistically learnable representation. Fine-tuned LLMs using specialized descriptors (mof2text) achieve performance comparable to graph-based models in identifying unreasonable MOFs. Importantly, these models extend beyond black-box classification by generating diagnostic rationales for likely error sources, including abnormal bonding, connectivity, and charge states, as well as error-category predictions for annotated datasets. This work establishes chemically informed textualization as the key step that transforms LLMs from generic text models into practical and explainable tools for curating MOF databases.

大模型材料科学可解释性结构验证

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