異丙醇—丙酮—氫氣化學熱泵中丙酮加氫反應選擇性研究

淮秀蘭 許閩

摘 要：采用實驗與理論相結合的方法，對高溫丙酮加氫反應副產物的產生路徑和機理進行了系統深入研究。反應動力學實驗發現高溫丙酮加氫反應的主要產物為裂解產物，主要是一氧化碳和甲烷?？账佟⒎磻獪囟群蛪毫Φ脑黾邮贡D化率降低，同時異丙醇反應選擇性降低，裂解產物選擇性增加；提高氫氣流量可以使丙酮轉化率增大，同時異丙醇反應選擇性增加，裂解產物選擇性降低；獲得了可以預測反應選擇性的反應動力學方程。通過密度泛函理論計算了副產物的產生路徑，發現丙酮的烯醇化是丙酮分解產物產生的源頭，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。

關鍵詞：化學熱泵 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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