Development of reaction-separation dual-functional membrane reactors for the facile synthesis of sustainable chemicals

开发用于可持续化学品简易合成的反应分离双功能膜反应器：在本研究项目中，我们专注于开发反应分离双功能膜反应器，以CO2为碳源，用于DME，DMC和MeOH等可持续化学品的简易合成。温室气体CO2将越来越多地从几个来源被隔离，特别是从发电站的废气，从水泥和钢铁工业。CO2是一种廉价、丰富、无毒、可再生的资源，可用于合成可持续发展的化学品。特别地，CO2可以代替CO用作合成二甲醚（DME）、碳酸二甲酯（DMC）或甲醇（MeOH）的起始碳化学品：（iv）2 CO2 + 6 H2至DME + 3 H2O 50巴，200至300 ℃（v）CO2 + 2 MeOH至DMC + H2O 50巴，100至200 ℃（vi）CO2 + 3 H2至MeOH + H2O 50巴，在这些反应中，产物水对催化剂的活性有害。水的去除也有利于上述反应克服平衡限制。反应分离双功能膜可以支持通过使用CO2作为起始碳源合成（i）DME、（ii）DMC和（iii）MeOH。水是一种临界直径为2.6 A的小分子，可以通过小孔亲水膜去除。超氧化物歧化酶（孔径为2.8A）和LTA（孔径为4.0A）具有较强的亲水性，是制备选择性水分离膜的有希望的候选者。金属-有机骨架（M0 F）膜，例如ZIF-8（3.4 A的孔径）和ZIF-90（3.5 A的孔径）也允许脱水。虽然分离膜的大部分准备工作将在宁波进行，但汉诺威将专注于催化层的沉积。反应（i）和（ii）将在宁波进行测试，反应（iii）将在汉诺威进行测试。我们提交一份工作计划，明确责任和里程碑。宁波和汉诺威之间的博士生交流是有组织的，就像我们过去做的那样。在分离和催化中使用高达50 bar的高压膜反应器将是膜研究和将CO2加工成可持续化学品的开创性突破。

Development of reaction separation dual functional membrane reactors for the facile synthesis of sustainable chemicals: In this joint research project, we focus on the development of reaction separation dual-functional membrane reactors for facile synthesis of sustainable chemicals such as DME, DMC, and MeOH by using CO2 as carbon source. Greenhouse gases CO2 will be increasingly sequestrated from several sources, especially from the exhaust gas of electrical power stations, from cement and iron industry. CO2 is an inexpensive, abundant, nontoxic, and renewable resource for synthesis of sustainable chemicals. In particular, CO2 can be used instead of CO as starting carbon chemical for the synthesis of dimethylether (DME), dimethylcarbonate (DMC) or methanol (MeOH): (iv) 2 CO2 + 6 H2 to DME + 3 H2O 50 bar, 200 to 300°C (v) CO2 + 2 MeOH to DMC + H2O 50 bar, 100 to 200°C (vi) CO2 + 3 H2 to MeOH + H2O 50 bar, 100 to 200°C In these reactions, the product water is harmful to the activity of the catalysts. The removal of water is also beneficial for the above reactions to overcome the equilibrium limitation. Reaction separation dual functional membranes can support the synthesis of (i) DME, (ii) DMC, and (iii) MeOH by using CO2 as starting carbon source. Water is a small molecule with 2.6 A critical diameter and can be removed by small-pore hydrophilic membranes. Zeolite SOD (pore size of 2.8 A) and LTA (pore size of 4.0 A) with strong hydrophilicity are promising candidates for the fabrication of selective water-separation membranes. Also metal-organic frameworks (MOF) membranes, such as ZIF-8 (pore size of 3.4 A) and ZIF-90 (pore size of 3.5 A) allow dehydration. While most of the preparation work of the separation membrane will be made in Ningbo, Hannover will focus on the deposition of the catalytic layer. The reaction (i) and (ii) will be tested in Ningbo, reactions (iii) in Hannover. We submit a Working Plan with clear responsibilities and milestones. The exchange of the PhD students between Ningbo and Hannover is organized, as we did in the past. The use of a high-pressure membrane reactor up to 50 bar in separation and catalysis will be a pioneering breakthrough in membrane research and in the processing CO2 to sustainable chemicals.