解决生成催化剂表面后找不到对应母体晶体的问题,实现高精度检索。
CatRetriever: Contrastive Representation Learning for Slab-to-Bulk Retrieval in Generative Catalyst Discovery
- 通过对比学习将表面与体相结构映射到同一潜在空间,实现精准匹配。
- 在分布内和外数据上,检索准确率R@1超91%,R@3超98%。
- 适用于需要结构兼容性和吸附能匹配的催化材料发现任务。
逆向设计是高效探索庞大化学空间以发现目标性能新材料的数据驱动新范式。在异质催化领域,表面生成模型已能直接生成催化剂表面-吸附物结构,但通常仅在晶块(slab)层面操作,无法提供对应的母体体相结构,导致难以评估形成能、表面能、晶格对称性及可合成性等依赖体相性质。本文将此缺失的晶块到体相关联问题视为检索任务,提出CatRetriever——一种对比表示学习模型,可在共享潜在空间中对齐晶块与体相晶体表示。从晶块查询出发,该模型在分布内与外测试集上均实现R@1 > 91%、R@3 > 98%的检索准确率。进一步,我们拓展框架为面向吸附能的体相发现流程,结合体相检索、生成搜索空间扩展与吸附能分布分析,通过结构兼容性与多表面环境下的目标吸附能范围覆盖能力双重评估候选材料。该方法为连接生成式催化剂模型与物理合理、吸附能兼容的体相催化剂发现提供了可扩展路径。
原文摘要 · Abstract (English)
Inverse design is an emerging data-driven paradigm for efficiently navigating vast chemical spaces to discover new materials with targeted properties, and in the context of heterogeneous catalysis, surface generative models have recently advanced this goal by directly generating catalyst surface-adsorbate structures. However, these models typically operate at the slab level and do not provide the corresponding parent bulk structure, making it difficult to assess bulk-dependent properties such as formation energy, surface energy, crystallographic symmetry, and synthesizability. Here, we address this missing slab-to-bulk connection as a retrieval problem and introduce CatRetriever, a contrastive representation learning model that aligns slab and bulk crystal representations in a shared latent space. From a slab query, CatRetriever accurately retrieves plausible parent bulk candidates with R@1 > 91% and R@3 > 98% on both the in-distribution and holdout evaluation sets. We further extend the CatRetriever framework into an adsorption energy targeted bulk discovery pipeline that combines bulk retrieval, generative search space expansion, and adsorption energy distribution analysis. This workflow evaluates candidates by both structural compatibility with the query slab and their ability to access the target adsorption energy range across diverse surface environments. CatRetriever therefore provides a scalable route for connecting catalyst generative models with physically plausible and adsorption energy compatible bulk catalyst discovery.
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