本文關鍵詞：銀、鈰雙金屬改性的微-介孔Y分子篩制備及其吸附脫硫性能　出處：《東北石油大學》2017年碩士論文　論文類型：學位論文

  更多相關文章： 吸附脫硫 金屬改性 孔道調變 動力學 熱力學

【摘要】：采用連續(xù)脫鋁脫硅過程和液相離子交換Ag、Ce離子成功制備了微-介孔meso-AgCeY吸附劑,并使用比表面積測定(BET)、X射線衍射(XRD)、吡啶紅外(Py-IR)、傅立葉變換紅外(FT-IR)、掃描電子顯微鏡(SEM)、X射線光電子能譜(XPS)和透射電子顯微鏡(TEM)等手段對分子篩吸附劑進行了物化性質表征。以含有不同競爭組分(甲苯或環(huán)己烯)的模擬油為原料,通過靜態(tài)吸附脫硫法考察了制備條件對吸附劑脫硫性能的影響,通過固定床吸附脫硫法探究了吸附劑選擇性吸附脫硫的性能,考察了吸附劑的再生能力,并研究了微-介孔meso-AgCeY吸附噻吩的等溫吸附和吸附動、熱力學。結果表明:(1)微-介孔meso-NaY分子篩適宜的孔調變條件為EDTA處理濃度為0.2mol·L~(-1),EDTA處理時間為6 h,NaOH處理濃度為0.8 mol·L~(-1),NaOH處理時間為30 min;(2)適宜的液相離子交換條件為Ce/Ag摩爾比為7.5,Ce離子交換時間為24 h,焙燒溫度為500℃;(3)吸附劑的最佳吸附條件為吸附時間為20 min,吸附溫度為50℃;(4)隨著原料油中甲苯濃度提高,未進行孔調變的AgCeY和孔調變后的微-介孔meso-AgCeY分子篩吸附劑的吸附選擇性均有明顯下降,但當甲苯濃度為16.6 vol.%時,AgCeY喪失了選擇性脫硫能力,而微-介孔meso-AgCeY仍然保留了一定的吸附能力;與甲苯類似,以環(huán)己烯為競爭組分的一系列模擬油,隨著環(huán)己烯濃度的提高,兩種吸附劑的吸附選擇性有明顯下降,但當環(huán)己烯濃度為15.8 vol.%時,AgCeY喪失了選擇性脫硫能力,而微-介孔meso-AgCeY仍然保留了一定的吸附能力。表明孔道調變能顯著提高吸附劑的選擇性吸附能力,微-介孔meso-AgCeY的介孔結構會削弱“微孔填充效應”,能夠在高濃度競爭組分存在的模擬油中保持良好的吸附脫硫選擇性;(5)微-介孔meso-AgCeY吸附劑具有良好的再生性能,經乙醇洗滌、烘干、焙燒5次再生后,脫硫性能僅下降了6.3%;(6)微-介孔meso-AgCe Y對噻吩的吸附符合Langmuir模型;微-介孔meso-AgCeY吸附噻吩的過程可以用準一級速率方程和Langmuir模型描述;吸附是自發(fā)的、放熱的過程。
[Abstract]:Micromesoporous meso-AgCeY adsorbents were successfully prepared by continuous desilication and liquid-phase ion exchange. X-ray diffraction (XRD), pyridine infrared (Py-IR), Fourier transform infrared (FT-IR), scanning electron microscopy (SEM). The physicochemical properties of molecular sieve adsorbents were characterized by means of X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM). Different competitive components (toluene or cyclohexene) were used to characterize molecular sieve adsorbents. The simulated oil is used as raw material. The influence of preparation conditions on the desulfurization performance of adsorbent was investigated by static adsorption desulfurization method. The performance of selective adsorption desulfurization of adsorbent was investigated by fixed-bed adsorption desulfurization method, and the regeneration ability of adsorbent was investigated. The isothermal adsorption and adsorption of thiophene on micromesoporous meso-AgCeY were studied. Thermodynamics. The results show that the suitable pore modification conditions for micromesoporous meso-NaY molecular sieve are 0.2mol 路L ~ (-1) EDTA treatment concentration. The treatment time of EDTA was 0. 8 mol 路L ~ (-1) and NaOH was 0. 8 mol 路L ~ (-1). The suitable liquid phase ion exchange conditions are as follows: the molar ratio of Ce/Ag is 7.5%, the exchange time of ce is 24 h, and the calcination temperature is 500 鈩，

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