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首页> 外文期刊>ACS Sustainable Chemistry & Engineering >Hydrogenation of Carbon Monoxide into Formaldehyde in Liquid Media
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Hydrogenation of Carbon Monoxide into Formaldehyde in Liquid Media

机译：一氧化碳在液体介质中的加氢成甲醛

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Formaldehyde is a bulk chemical which is produced in excess of 30 million tons per annum and is growing in demand. However, the current production process requires methanol production, which is oxidized in air to produce formaldehyde, which must then be absorbed into water. Our recent work introduced a novel method to produce formaldehyde through CO hydrogenation in the aqueous phase. However, the aqueous phase has certain limitations which must be overcome to make it commercially viable. By applying a deuterium labeling technique and investigating the potential intermediates, the reaction mechanism was established which showed that solvents play a vital role in determining the yield. Various solvents were used for formaldehyde production, and the highest formaldehyde yield was achieved by using pure methanol followed by methanol-water mixtures. Formaldehyde reacts with methanol and water to produce hemiacetal and methylene glycol, respectively, thereby shifting the equilibrium of CO hydrogenation toward formaldehyde production. Methanol and water stabilize the hemiacetal and methylene glycol molecules, respectively, via hydrogen bonding. The highest yield of formaldehyde in methanol solvent was found to be 15.58 mmol L~(-1) gcat -1 at 363 K and 100 bar, which is four times higher than our previous report. The liquid phase method shown here has the potential to be greener and more sustainable than the commercial processes because it operates at low temperatures and results in 100% selectivity toward formaldehyde with no CO2 generation.
机译：甲醛是一种大宗化学品，每年的产量超过3000万吨，并且需求不断增长。但是，当前的生产过程需要生产甲醇，甲醇在空气中被氧化生成甲醛，然后必须将甲醛吸收到水中。我们最近的工作介绍了一种通过在水相中进行CO加氢生产甲醛的新方法。但是，水相具有一定的局限性，必须使其克服才能使其在商业上可行。通过应用氘标记技术并研究潜在的中间体，建立了反应机理，该机理表明溶剂在确定产率中起着至关重要的作用。各种溶剂均用于甲醛生产，通过先后使用纯甲醇和甲醇-水的混合物，可以达到最高的甲醛收率。甲醛与甲醇和水反应分别生成半缩醛和亚甲基二醇，从而将CO加氢的平衡向甲醛生成转移。甲醇和水分别通过氢键稳定半缩醛和亚甲基二醇分子。在363 K和100 bar下，甲醇溶剂中甲醛的最高收率是15.58 mmol L〜（-1）gcat -1，是我们先前报告的四倍。此处显示的液相方法比工业方法具有更绿色，更可持续的潜力，因为它在低温下运行，并且对甲醛的选择性为100％，而不会产生CO2。

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