Towards environmentally benign capture and conversion: heterogeneous metal catalyzed CO2 hydrogenation in CO2 capture solvents,Green Chemistry

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Towards environmentally benign capture and conversion: heterogeneous metal catalyzed CO2 hydrogenation in CO2 capture solvents
Green Chemistry ( IF 9.3 ) Pub Date : 2020/01/06 , DOI: 10.1039/c9gc03449h
Jotheeswari Kothandaraman _{1,

2,

3,

4} , David J. Heldebrant _{1,

2,

3,

4}

Affiliation

The transformation of captured CO₂ into value-added chemicals to mitigate increasing CO₂ concentration in the atmosphere has gained significant attention recently. Though carbon capture and storage (CCS) is already being practiced in a few places, it suffers from energy-intensive CO₂ desorption and compression steps involved, which can be avoided in the carbon capture and utilization (CCU) approach. Herein, a selection of carbon capture solvents were screened to assess the reactivity of condensed-phase heterogeneous metal catalyzed hydrogenation of CO₂. Among the catalysts screened, the Cu/ZnO/Al₂O₃ catalyst was active for the one-pot CO₂ capture and conversion process to methanol using post and pre-combustion carbon capture solvents comprised of various amines and alcohols. Our findings indicate that formamides are less-reactive under our conditions in comparison with formate ester intermediates and a combination of 1° alcohols and amines gives the highest methanol yield. Screening volatile organic compound (VOC)-free alcohols and amines led us to an environmentally benign system of bio-derived and biodegradable chitosan and polyethylene glycol (PEG₂₀₀), which provide a moderate concentration of methanol (139.5 mmol L⁻¹) with the facile separation of volatile products (water and methanol). The chitosan/PEG₂₀₀ system was recycled three times, ultimately providing a promising VOC-free, biodegradable, bio-derived and recyclable CO₂ capture and conversion pathway.

中文翻译：

迈向环境友好的捕获和转化：在CO2捕获溶剂中多相金属催化的CO2加氢

将捕获的CO ₂转化为增值化学品以减轻大气中不断增加的CO ₂浓度近来引起了广泛关注。尽管碳捕集与封存（CCS）已经在一些地方进行了实践，但它涉及到能源密集型CO _2的解吸和压缩步骤，在碳捕集与利用（CCU）方法中可以避免这种情况。在此，筛选碳捕获溶剂的选择以评估冷凝相异相金属催化CO ₂加氢的反应性。在筛选出的催化剂中，Cu / ZnO / Al ₂ O ₃催化剂对一锅法CO ₂具有活性燃烧和燃烧后的碳捕获溶剂（包括各种胺和醇）将其捕获并转化为甲醇。我们的发现表明，与甲酸酯中间体相比，甲酰胺在我们的条件下反应性较低，并且1°醇和胺的组合可提供最高的甲醇收率。筛选不含挥发性有机化合物（VOC）的醇和胺，使我们建立了对环境有益的生物衍生和可生物降解的壳聚糖和聚乙二醇（PEG ₂₀₀）系统，该系统可提供中等浓度的甲醇（139.5 mmol L ^-1）和轻松分离挥发性产物（水和甲醇）。壳聚糖/ PEG ₂₀₀该系统被回收了三次，最终提供了一种有希望的无VOC，可生物降解，可生物来源和可回收的CO ₂捕获和转化途径。

更新日期：2020-02-13

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