H_(2)小分子原位调控负载型Ni_(x)Mo_(y)S@Al_(2)O_(3)用于加氢脱硫的研究

Supported Ni_(x)Mo_(y)S@Al_(2)O_(3) catalyst by in-situ H_(2)small molecule regulation for hydrodesulfurization

通过H_(2)气体小分子原位调控技术制得系列NiMoS-nH_(2)[n=0.5,1.0,1.4,2.0,为H_(2)压力(MPa)]催化剂,活性评价结果表明,2 MPa的H_(2)原位调控制得的NiMoS催化剂(NiMoS-2.0H_(2))具有最优的加氢脱硫活性;进一步制备具有介孔结构的Al_(2)O_(3)载体,并采用原位生长法,制得NiMoS-2.0H_(2)S@Al_(2)O_(3)负载型加氢脱硫催化剂,活性评价结果表明,负载型NiMoS-2.0H_(2)S@Al_(2)O_(3)较NiMoS-2.0H_(2)加氢脱硫性能显著提升,在温度240℃和压力2 MPa条件下,苯并噻吩脱除率高达73%,脱硫效率约为NiMoS-2.0H_(2)粉末催化剂的两倍。XRD、XPS、N_(2)吸附-脱附表征分析表明,负载型NiMoS-2.0H_(2)S@Al_(2)O_(3)具备超高的比表面积,可显著提高NiMoS-2.0H_(2)表面分散,是构成其高活性的重要原因。通过气体小分子原位调控及原位生长制备策略,成功开发一种新型高效非贵金属负载型加氢脱硫催化剂,研究结果可为其他高效加氢脱硫催化剂开发提供设计思路。

In this paper,a series of NiMoS-nH_(2)[n=0.5,1.0,1.4,2.0,H_(2)pressure(MPa)]catalysts was prepared using in-situ H_(2)gas small molecule control technology.The activity evaluation results showed that the NiMoS catalyst(NiMoS-2.0H_(2))obtained by in-situ control of 2 MPa H_(2)had the optimal hydrodesulfurization activity.The Al_(2)O_(3)support with mesoporous structure was further prepared and utilized during the in-situ synthesis of supported catalyst NiMoS-2.0H_(2)S@Al_(2)O_(3)for hydrodesulfurization.The activity evaluation results indicate that the supported NiMoS-2.0H_(2)S@Al_(2)O_(3)possesses significantly improved hydrodesulfurization performance than that of NiMoS-2.0H_(2)powder catalyst sample.Over NiMoS-2.0H_(2)S@Al_(2)O_(3),the removal of benzothiophene is as high as 73%,and the desulfurization efficiency is about twice of NiMoS-2.0H_(2)powder catalyst under the conditions of 240℃and 2 MPa.The XRD,XPS,N_(2)adsorption-desorption analysis showed that ultra-high specific surface area of loaded NiMoS-2.0H_(2)S@Al_(2)O_(3)can significantly improve the surface dispersion of NiMoS-2.0H_(2),which constitutes an important reason for its high activity.This study successfully developed a new type of high-efficiency non precious metal supported hydrodesulfurization catalyst through in-situ regulation of gas small molecules and in-situ growth preparation strategy.The research results of this paper can provide design ideas for the development of other high-efficiency hydrodesulfurization catalysts.