Optimizing accuracy and efficacy in data-driven materials discovery for the solar production of hydrogen
Optimizing accuracy and efficacy in data-driven materials discovery for the solar production of hydrogen
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DOI：
10.1039/d0ee02984j
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发表时间：
2021-03-11
影响因子：
32.5
通讯作者：
Dabo, Ismaila
中科院分区：
文献类型：
--
作者：
Xiong, Yihuang;Campbell, Quinn T.;Dabo, Ismaila
通过水分解生产氢燃料对于满足全球能源需求和减轻化石燃料运输的环境后果具有实际意义。已经提出水光电解作为用于产生氢的可行方法，条件是可以发现、大规模合成并成功部署具有超过10%的转化效率的稳定且廉价的光催化剂（Pinaud等人，能源环境。科学，2013，6，1983）。虽然许多第一性原理研究都集中在光催化剂的数据驱动发现上，但在缺乏系统实验验证的情况下，这些预测的成功率可能是有限的。我们解决这个问题，通过开发一个筛选程序与实验和理论之间的共同验证，以加快合成，表征和测试的计算预测，最理想的材料。从材料项目数据库中的70 150种化合物开始，拟议的协议产生了71种候选光催化剂，其中11种是合成为单相材料。实验证实了11种化合物中有6种具有产氢和良好的能带排列，其中最有前途的是碱金属和碱土金属铟酸盐和正铅酸盐。这项研究显示了一个非经验的，哈伯德校正的密度泛函理论方法的准确性，以预测带隙和带偏移的计算成本的一小部分的混合泛函，并概述了一个有效的策略，以确定太阳能制氢的光催化剂。
The production of hydrogen fuels, via water splitting, is of practical relevance for meeting global energy needs and mitigating the environmental consequences of fossil-fuel-based transportation. Water photoelectrolysis has been proposed as a viable approach for generating hydrogen, provided that stable and inexpensive photocatalysts with conversion efficiencies over 10% can be discovered, synthesized at scale, and successfully deployed (Pinaud et al., Energy Environ. Sci., 2013, 6, 1983). While a number of first-principles studies have focused on the data-driven discovery of photocatalysts, in the absence of systematic experimental validation, the success rate of these predictions may be limited. We address this problem by developing a screening procedure with co-validation between experiment and theory to expedite the synthesis, characterization, and testing of the computationally predicted, most desirable materials. Starting with 70 150 compounds in the Materials Project database, the proposed protocol yielded 71 candidate photocatalysts, 11 of which were synthesized as single-phase materials. Experiments confirmed hydrogen generation and favorable band alignment for 6 of the 11 compounds, with the most promising ones belonging to the families of alkali and alkaline-earth indates and orthoplumbates. This study shows the accuracy of a nonempirical, Hubbard-corrected density-functional theory method to predict band gaps and band offsets at a fraction of the computational cost of hybrid functionals, and outlines an effective strategy to identify photocatalysts for solar hydrogen generation.