Towards environmentally benign capture and conversion: heterogeneous metal catalyzed CO2 hydrogenation in CO2 capture solvents
Towards environmentally benign capture and conversion: heterogeneous metal catalyzed CO2 hydrogenation in CO2 capture solvents
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DOI：
10.1039/c9gc03449h
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发表时间：
2020-02-07
期刊：
影响因子：
9.8
通讯作者：
Heldebrant, David J.
中科院分区：
文献类型：
--
作者：
Kothandaraman, Jotheeswari;Heldebrant, David J.
将捕获的二氧化碳转化为增值化学品以减轻大气中不断增加的二氧化碳浓度最近受到了极大的关注。尽管碳捕集与封存（CCS）已经在一些地方得到了实践，但它所涉及的能源密集型二氧化碳解吸和压缩步骤是可以在碳捕集与利用（CCU）方法中避免的。本文筛选了几种碳捕获溶剂，以评估冷凝相非均相金属催化CO2加氢的反应性。在所筛选的催化剂中，Cu/ZnO/Al2O3催化剂在燃烧后和燃烧前碳捕集溶剂由各种胺和醇组成的情况下，对一锅CO2捕集转化为甲醇具有活性。我们的研究结果表明，在我们的条件下，与甲酸酯中间体相比，甲酰胺的反应性较低，1度醇和胺的组合产生了最高的甲醇收率。通过筛选不含挥发性有机化合物（VOC）的醇类和胺类化合物，我们得到了一种由生物衍生和可生物降解的壳聚糖和聚乙二醇（PEG(200)）组成的环境友好型体系，该体系可提供中等浓度的甲醇（139.5 mmol L-1），并易于分离挥发性产物（水和甲醇）。壳聚糖/PEG（200）体系可循环利用三次，最终提供了一种无voc、可生物降解、生物衍生和可循环利用的CO2捕获和转化途径。
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 degrees 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 (PEG(200)), which provide a moderate concentration of methanol (139.5 mmol L-1) with the facile separation of volatile products (water and methanol). The chitosan/PEG(200) system was recycled three times, ultimately providing a promising VOC-free, biodegradable, bio-derived and recyclable CO2 capture and conversion pathway.