Density functional theory (DFT) is widely used to connect atomic structure with catalytic behavior, but computational heterogeneous catalysis studies often require long workflows that are costly, iterative, and sensitive to setup choices. Besides the intrinsic cost and accuracy limits of first-principles calculations, practical workflow issues such as keeping references consistent, preparing many related inputs, recovering from failed runs on computing clusters, and maintaining a complete record of what was done, can slow down projects and make results difficult to reproduce or extend. Here we present CatMaster, a large-language-model (LLM)-driven agent system that turns natural language requests into complete calculation workspaces, including structures, inputs, outputs, logs, and a concise run record. CatMaster maintains a persistent project record of key facts, constraints, and file pointers to support inspection and restartability. It is paired with a multi-fidelity tool library that covers rapid surrogate relaxations and high-fidelity DFT calculations for validation when needed. We demonstrate CatMaster on four demonstrations of increasing complexity: an O2 spin-state check with remote execution, BCC Fe surface energies with a protocol-sensitivity study and CO adsorption site ranking, high-throughput Pt--Ni--Cu alloy screening for hydrogen evolution reaction (HER) descriptors with surrogate-to-DFT validation, and a demonstration beyond the predefined tool set, including equation-of-state fitting for BCC Fe and CO-FeN4-graphene single-atom catalyst geometry preparation. By reducing manual scripting and bookkeeping while keeping the full evidence trail, CatMaster aims to help catalysis researchers focus on modeling choices and chemical interpretation rather than workflow management.

翻译：密度泛函理论（DFT）被广泛用于关联原子结构与催化行为，但计算多相催化研究通常需要耗时、迭代且对设置选择敏感的长流程工作流。除了第一性原理计算固有的成本与精度限制外，实际工作流中的诸多问题——如保持参考文献一致性、准备大量相关输入文件、从计算集群的失败运行中恢复、以及维护完整的操作记录——均会拖慢项目进度，并使结果难以复现或扩展。本文提出CatMaster，一个由大语言模型（LLM）驱动的智能体系统，能够将自然语言请求转化为完整的计算工作空间，包含结构、输入、输出、日志及简明的运行记录。CatMaster维护包含关键事实、约束条件和文件指针的持久化项目记录，以支持检查与可重启性。该系统配有一个多精度工具库，涵盖快速代理弛豫计算和用于必要验证的高精度DFT计算。我们通过四个复杂度递增的案例展示CatMaster的功能：基于远程执行的O2自旋态校验、包含协议敏感性研究的BCC Fe表面能计算与CO吸附位点排序、面向氢析出反应（HER）描述符的高通量Pt-Ni-Cu合金筛选（辅以代理模型至DFT的验证）、以及超越预设工具集的演示（包括BCC Fe的状态方程拟合和CO-FeN4-石墨烯单原子催化剂几何结构制备）。通过减少手动脚本编写与记录工作，同时保留完整的证据链，CatMaster旨在帮助催化研究者聚焦于建模选择与化学机理分析，而非工作流管理。