CAJ | 학술논문

采用共浸渍法制备了P/Ni摩尔比为2的Ni_2P/SBA-15,再通过二次浸渍引入助剂Mo制得Mo-Ni_2P/SBA-15,将它调制成活件胶后均匀涂敷于预处理后的载体表面,干燥焙烧后在氢气流中采用程序升温还原法,制备了一系列Mo-Ni_2P/SBA-15/堇青石整体式催化剂.采用X射线衍射、N_2吸附-脱附和X射线光电子能谱对催化剂结构进行了表征,以二苯并噻吩为模型含硫化合物,考察了催化剂的加氢脱硫件能.结果表明,Mo的加入增大了催化剂的比表面积,在催化剂表面形成了MoNiP_2,且Ni_2P为主要活性物相.Mo在催化剂表而主要以Mo~(6+)和Mo~(δ+)形式存在;当w(Mo)=4.2%时,n(Mo)/n(Ni+Mo)=0.18的整体式催化剂上二苯并噻吩的转化率最高,且在较低反应温度时以直接脱硫机理为主,而较高反应温度时以加氢脱硫机理为主.
채용공침지법제비료P/Ni마이비위2적Ni_2P/SBA-15,재통과이차침지인입조제Mo제득Mo-Ni_2P/SBA-15,장타조제성활건효후균균도부우예처리후적재체표면,간조배소후재경기류중채용정서승온환원법,제비료일계렬Mo-Ni_2P/SBA-15/근청석정체식최화제.채용X사선연사、N_2흡부-탈부화X사선광전자능보대최화제결구진행료표정,이이분병새분위모형함류화합물,고찰료최화제적가경탈류건능.결과표명,Mo적가입증대료최화제적비표면적,재최화제표면형성료MoNiP_2,차Ni_2P위주요활성물상.Mo재최화제표이주요이Mo~(6+)화Mo~(δ+)형식존재;당w(Mo)=4.2%시,n(Mo)/n(Ni+Mo)=0.18적정체식최화제상이분병새분적전화솔최고,차재교저반응온도시이직접탈류궤리위주,이교고반응온도시이가경탈류궤리위주.
A series of Mo-Ni_2P/SBA-15/cordierite monolithic catalysts with different Mo contents were prepared by dipping a sol containing nickel phosphide precursors (prepared by impregnating nickel nitrate, diammonium hydrogen phosphate, and ammonium into SBA-15) on a pretreated cordierite support followed by temperature-programmed reduction in a H2 flow. The structure of the catalysts was characterized by N2 adsorption-desorption, X-ray diffraction, and X-ray photoelectron spectroscopy. The catalytic performance of the catalysts for hydrode-sulfurization (HDS) was evaluated in a fixed-bed microreactor using dibenzothiophene as the model compound. The results indicated that the addition of Mo increased the surface area of the catalysts. Ni_2P particles were the active phase, and there was the MoNiP_2 phase when Mo was added. The valence states of Mo were mainly Mo~(6+) and Mo~(δ+). The Mo-NiEP/SBA-15/cordierite monolithic catalysts with w(Mo) = 4.2%and n(Mo)/n(Ni+Mo)= 0.18 had perfect HDS catalytic performance. When Mo was added, the hydrodesulfurization route was the dominant path at high temperature, and direct desulfurization route at low temperature.