淮秀蘭 許閩

摘 要：采用實(shí)驗(yàn)與理論相結(jié)合的方法，對(duì)高溫丙酮加氫反應(yīng)副產(chǎn)物的產(chǎn)生路徑和機(jī)理進(jìn)行了系統(tǒng)深入研究。反應(yīng)動(dòng)力學(xué)實(shí)驗(yàn)發(fā)現(xiàn)高溫丙酮加氫反應(yīng)的主要產(chǎn)物為裂解產(chǎn)物，主要是一氧化碳和甲烷。空速、反應(yīng)溫度和壓力的增加使丙酮轉(zhuǎn)化率降低，同時(shí)異丙醇反應(yīng)選擇性降低，裂解產(chǎn)物選擇性增加；提高氫氣流量可以使丙酮轉(zhuǎn)化率增大，同時(shí)異丙醇反應(yīng)選擇性增加，裂解產(chǎn)物選擇性降低；獲得了可以預(yù)測反應(yīng)選擇性的反應(yīng)動(dòng)力學(xué)方程。通過密度泛函理論計(jì)算了副產(chǎn)物的產(chǎn)生路徑，發(fā)現(xiàn)丙酮的烯醇化是丙酮分解產(chǎn)物產(chǎn)生的源頭，并指出采用PtCu催化劑并降低催化劑酸性可以改善丙酮加氫選擇性。

關(guān)鍵詞：化學(xué)熱泵 丙酮加氫 選擇性 密度泛函理論 鉑銅合金

Abstract：The reaction pathway and mechanism of high-temperature acetone hydrogenation was studied by using combined experimental and computational method. The experimental results showed that the main side reaction is the cracking of the acetone and the main by-products are CO and methane. The increase of the space velocity， temperature and pressure decreases the conversion and selectivity of acetone， and the increment of the hydrogen flow rate increases the conversion and selectivity of acetone. The kinetic equations that can predict the selectivity of acetone was obtained. In addition， the DFT calculations suggested that the keto-enol isomerization is origin of the decomposition of acetone. And then the selectivity can be improved by using PtCu alloy catalyst and decreasing the acidic functions of the catalyst.

Key Words：Chemical heat pump；Acetone hydrogenation；Selectivity；DFT；PtCu alloy

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