Квантово-химическое моделирование адсорбции водорода в порах: исследование методами DFT, SAPT0 и IGM

Привлекательность водорода как универсального энергоносителя определяет значительный интерес к нему со стороны прикладной химии. Одной из центральных проблем, которую необходимо решить для перехода к водородной энергетике, является проблема его хранения. Физическая адсорбция водорода в порах – это практически важный и эффективный метод хранения водорода. Среди существующих адсорбирующих водород материалов углеродные наноструктуры обладают рядом преимуществ: высокой адсорбционной емкостью, значительной прочностью и низким весом. В данной работе с помощью современных методов квантовой химии (DFT, SAPT0, IGM) изучена адсорбция молекулярного водорода в ряде модельных щелевидных углеродных микропор с расстоянием между стенками d = 4–10 Å, включая введение молекулы H₂ в пору, наполнение поры этими молекулами и изучение взаимодействий между молекулами H₂ внутри поры. Установлено, что в зависимости от величины параметра d, адсорбированные молекулы водорода образуют один (d = 6, 7 Å) или два слоя (d = 8, 9, 10 Å) внутри поры. В то же самое время для пор с малым d наблюдались высокие потенциальные барьеры введения H₂ в пору. Разложение энергии взаимодействия на компоненты показало, что дисперсионные взаимодействия дают основной вклад в энергию притяжения (72–82%), причем с увеличением числа молекул H₂, адсорбированных в поре, их значимость снижается (вплоть до 61%), а вклад в межмолекулярное притяжение электростатических и индукционных взаимодействий растет. Также были определены значения гравиметрической плотности (GD) для пор с d = 6, 7, 8, 9, 10 Å, которые равны соответственно 1,98; 2,30; 2,93; 3,25; 4,49 вес.%. Предполагается, что особенности адсорбции водорода в порах, выявленные в этой работе, будут способствовать применению углеродных пористых структур как среды для хранения водорода.

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