Determining desired sorbent properties for proton-coupled electron transfer-controlled CO2 capture using an adaptive sampling-refined classifier
Determining desired sorbent properties for proton-coupled electron transfer-controlled CO2 capture using an adaptive sampling-refined classifier
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DOI：
10.1016/j.ces.2023.118673
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发表时间：
2023-03
影响因子：
4.7
通讯作者：
Jonathan Boualavong;Kostas Papakonstantinou;C. Gorski
中科院分区：
文献类型：
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作者：
Jonathan Boualavong;Kostas Papakonstantinou;C. Gorski
电化学CO2捕集技术已被发现比热分离的工业标准消耗更少的能量，但它们的实际应用要求它们也以可比的速率运行。优化低能量需求和高捕获率是复杂的权衡两个目标和许多可操纵的溶液化学变量，包括物种类型和浓度。在这里，我们计算确定的解决方案的化学是最有可能超越热分离的能量需求和捕获率的电化学捕获驱动的质子耦合电子转移反应，通过使用自适应采样轮廓估计方法。这种方法通过选择信息量最大的条件进行测试，提供了高置信度的推断，只需很少的模拟运行。我们发现，适度的基本pKa值的还原形式的氧化还原活性化合物是最重要的变量，低能量和高速率CO2捕获。
Electrochemical CO2capture technologies have been found to consume less energy than the industry standard of thermal separations, but their real-world applicability requires that they also operate at comparable rates. Optimizing for both low energy demands and high capture rates is complicated by trade-offs between the two objectives and the many manipulable solution chemistry variables, including species type and concentration. Here, we computationally identified the solution chemistries that are most likely to outperform thermal separations in both energy demand and capture rate for electrochemical capture driven by proton-coupled electron transfer reactions by using an adaptive sampling contour estimation method. This approach provided high confidence inferences with few simulation runs by selecting the most informative conditions to test. We found that moderately basic pKavalues of the reduced form of the redox-active compound were the most important variables for low energy and high rate CO2capture.