SI2-CHE: Collaborative Research: Developing First Principles Monte Carlo Methods for Reactive Phase and Sorption Equilibria in the CP2k Software Suite

在分子尺度上探测反应平衡和阐明反应途径是化学科学中持久而难以捉摸的目标。在这里，我们建议通过添加新的功能来改变领先的第一性原理代码CP2K的预测能力，这将大大提高其预测相平衡的能力，并从化学反应中获得详细的分子见解。这个由化学家、化学工程师和计算机科学家组成的国际化团队在开发、优化和应用CP2K代码方面拥有无与伦比的经验，在实施和利用新型模拟方法方面也有着良好的记录。成功的实施将是变革性的理解和预测自由能景观和产品产量的反应多相系统，并确定最佳的反应条件和分离过程的可持续化学。EPSRC和NSF已将应对化学科学重大挑战的呼吁确定为具有国家重要性的关键战略举措。这里提出的工作支持化学领域的所有部门，特别是EPSRC优先考虑的催化主题。

Probing reactive equilibria at the molecular scale and elucidating reaction pathways are enduring and elusive goals in the chemical sciences. Here, we propose to transform the predictive capabilities of a leading first principles code, CP2K, by adding new functionality that will dramatically enhance its ability to predict phase equilibria and extricate detailed molecular insights underlying chemical reactions. The carefully assembled, international team of chemists, chemical engineers and computer scientists has unrivalled experience in developing, optimizing and applying the CP2K code and a proven record of implementing and exploiting novel simulation approaches. Successful implementation will be transformative for understanding and predicting free energy landscapes and product yields for reactive multi-phase systems and for identifying optimal reaction conditions and separation processes for sustainable chemistry. The call to address grand challenges in the chemical sciences has been identified by EPSRC and NSF as a key, strategic initiative of national importance. The work proposed here underpins all sectors of the chemistry field, and in particular the EPSRC prioritised theme of Catalysis.