從中科院獲悉，近日，中國(guó)科學(xué)院大連化學(xué)物理研究所甲醇制烯烴國(guó)家工程實(shí)驗(yàn)室劉中民、魏迎旭團(tuán)隊(duì)在甲醇制烯烴初始C-C鍵生成機(jī)理研究方面取得新進(jìn)展。以“熱點(diǎn)文章”形式發(fā)表在《德國(guó)應(yīng)用化學(xué)》。 甲醇制烯烴國(guó)家工程實(shí)驗(yàn)室一直堅(jiān)持應(yīng)用研究與基礎(chǔ)研究并重，不但在甲醇制烯烴(MTO)過程工業(yè)化方面取得巨大成功，而且長(zhǎng)期致力于該化學(xué)過程中的基礎(chǔ)科學(xué)問題研究。雖然MTO過程穩(wěn)態(tài)反應(yīng)階段的間接機(jī)理已形成廣泛的共識(shí)，但MTO反應(yīng)中從C1物種甲醇或者二甲醚生成第一個(gè)C-C鍵的反應(yīng)一直是C1化學(xué)中極具挑戰(zhàn)性和爭(zhēng)議性的課題。由于轉(zhuǎn)化發(fā)生在反應(yīng)的最初始階段，難以捕獲中間物種，一直以來所提出的反應(yīng)機(jī)理缺乏直接證據(jù)。該 項(xiàng)工作中，研究人員通過在線監(jiān)測(cè)最初始反應(yīng)階段，推測(cè)初始烯烴來源于催化劑表面C1吸附物種的直接轉(zhuǎn)化;隨后通過催化劑液氮淬冷和固體核磁表征，確定了催化劑上最初始反應(yīng)階段存在的表面C1吸附物種(甲醇和二甲醚)和C1活性物種(表面甲氧基和三甲基氧鎓離子);進(jìn)一步通過原位固體核磁研究，在真實(shí)甲醇轉(zhuǎn)化反應(yīng)條件下，成功捕捉到二甲醚C-H鍵活化后生成的類亞甲氧基物種，由此獲取了C1物種活化生成第一個(gè)C-C鍵的直接證據(jù);在此基礎(chǔ)上提出了初始烯烴生成的反應(yīng)路徑——表面甲氧基/三甲基氧鎓離子協(xié)助甲醇/二甲醚活化轉(zhuǎn)化的協(xié)同反應(yīng)機(jī)理。這是首次在MTO反應(yīng)過程中原位觀測(cè)到C1物種的初始活化和轉(zhuǎn)化，這一發(fā)現(xiàn)將關(guān)聯(lián)甲醇初始轉(zhuǎn)化的直接機(jī)理和高效轉(zhuǎn)化階段的間接機(jī)理，建立甲醇轉(zhuǎn)化反應(yīng)完整的反應(yīng)歷程。 此前在MTO反應(yīng)穩(wěn)定階段烴池(Hydrocarbon Pool)機(jī)理的研究中，研究人員曾直接捕捉到最為重要的反應(yīng)中間物種——苯基和環(huán)戊烯基碳正離子中間體，并確定了分子篩催化甲醇制烯烴的催化循環(huán)途徑。這些工作豐富了C1催化化學(xué)的基本理論，也對(duì)MTO的工業(yè)應(yīng)用具有重要的促進(jìn)和支撐作用。
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甲醇制烯烴反應(yīng)機(jī)理研究取得新進(jìn)展
Source： Time：2017-06-22 10:32:00 views：
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