CAJ | 학술논문

采用等体积浸渍法制备了 1% AuCl3/AC 催化剂,探究了硫化氢(H2S)为毒物对乙炔氢氯化反应中催化剂催化活性的影响及失活机理.催化活性测试结果表明,以 H2S 为毒物可导致乙炔氢氯化反应中的 AuCl3/AC 催化剂的失活,且是一个不可逆过程;程序升温还原(TPR)和 X 射线光电子能谱(XPS)分析结果表明,H2S 的加入可有效地加快 Au3+还原为 Au0;透射电镜能谱(TEM-EDX)观测分析形成的 Au-S 化合物也可导致催化剂失活,即随着 H2S 量的增大,更多的 Au3+被还原为 Au0,且形成的 Au-S 化合物覆盖在活性位点,使有效的活性组分降低进而导致 AuCl3/AC 催化剂失活.
채용등체적침지법제비료 1% AuCl3/AC 최화제,탐구료류화경(H2S)위독물대을결경록화반응중최화제최화활성적영향급실활궤리.최화활성측시결과표명,이 H2S 위독물가도치을결경록화반응중적 AuCl3/AC 최화제적실활,차시일개불가역과정;정서승온환원(TPR)화 X 사선광전자능보(XPS)분석결과표명,H2S 적가입가유효지가쾌 Au3+환원위 Au0;투사전경능보(TEM-EDX)관측분석형성적 Au-S 화합물야가도치최화제실활,즉수착 H2S 량적증대,경다적 Au3+피환원위 Au0,차형성적 Au-S 화합물복개재활성위점,사유효적활성조분강저진이도치 AuCl3/AC 최화제실활.
A study about poisoning effect of hydrogen sulfide (H2S) on the catalytic performance of AuCl3/AC during acetylene hydrochlorination deactivation is described and discussed. 1% AuCl3/AC catalyst is prepared by an incipient wetness impregnation technique. The activity tests demonstrate that H2S poisoning results in the rapid and irreversible deactivation of AuCl3/AC catalyst in acetylene hydrochlorination. Temperature-programmed reduction (TPR) and X-ray photoelectron spectra (XPS) show that H2S addition can effectively accelerate active Au3+ reduction to metallic Au0. The formation of metal sulfide may also be another reason for catalyst deactivation in the presence of H2S, which is supported by transmission electron microscopy (TEM) and energy dispersion X-ray spectrometer (EDX) techniques. In other words, with the increase of H2S added to the feed gases, the content of Au3+ is greatly reduced to metallic Au0. Moreover, the active sites are covered with Au-S compound. Both of them could reduce the effective active component, leading to the deactivation of the AuCl3/AC catalyst.