物理化学学报
物理化學學報
물이화학학보
ACTA PHYSICO-CHIMICA SINICA
2014年
6期
1148-1154
,共7页
陈世萍%王伟明%刘迎伟%魏育才%袁成龙%方维平%杨意泉
陳世萍%王偉明%劉迎偉%魏育纔%袁成龍%方維平%楊意泉
진세평%왕위명%류영위%위육재%원성룡%방유평%양의천
ZSM-5%过渡金属%甲硫醚%甲硫醇
ZSM-5%過渡金屬%甲硫醚%甲硫醇
ZSM-5%과도금속%갑류미%갑류순
ZSM-5%Transition metal%Dimethyl sulfide%Methanethiol
负载过渡金属的ZSM-5催化剂用于催化甲硫醚(DMS)转化成甲硫醇(MT)的反应.实验结果表明,催化剂的甲硫醚转化率提高和甲硫醇选择性降低的趋势一样,都是以下顺序:Co/ZSM-5>Mo/ZSM-5>Ni/ZSM-5>W/ZSM-5.表征结果表明,由于过渡金属阳离子(W6+、Ni2+、Co3+、Mo6+)比Al3+活泼,而改性过程中W6+、Ni2+、Co3+、Mo6+分别代替了部分Al3+,使得改性催化剂对DMS和MT的化学吸附作用更强.过渡金属的引入使得ZSM-5总酸度增强,提高了C-S键的裂解能力,从而改进了催化转化DMS的能力.研究结果发现,在转化DMS的过程中,金属活性位和酸性位之间通过强的协同效应起作用.
負載過渡金屬的ZSM-5催化劑用于催化甲硫醚(DMS)轉化成甲硫醇(MT)的反應.實驗結果錶明,催化劑的甲硫醚轉化率提高和甲硫醇選擇性降低的趨勢一樣,都是以下順序:Co/ZSM-5>Mo/ZSM-5>Ni/ZSM-5>W/ZSM-5.錶徵結果錶明,由于過渡金屬暘離子(W6+、Ni2+、Co3+、Mo6+)比Al3+活潑,而改性過程中W6+、Ni2+、Co3+、Mo6+分彆代替瞭部分Al3+,使得改性催化劑對DMS和MT的化學吸附作用更彊.過渡金屬的引入使得ZSM-5總痠度增彊,提高瞭C-S鍵的裂解能力,從而改進瞭催化轉化DMS的能力.研究結果髮現,在轉化DMS的過程中,金屬活性位和痠性位之間通過彊的協同效應起作用.
부재과도금속적ZSM-5최화제용우최화갑류미(DMS)전화성갑류순(MT)적반응.실험결과표명,최화제적갑류미전화솔제고화갑류순선택성강저적추세일양,도시이하순서:Co/ZSM-5>Mo/ZSM-5>Ni/ZSM-5>W/ZSM-5.표정결과표명,유우과도금속양리자(W6+、Ni2+、Co3+、Mo6+)비Al3+활발,이개성과정중W6+、Ni2+、Co3+、Mo6+분별대체료부분Al3+,사득개성최화제대DMS화MT적화학흡부작용경강.과도금속적인입사득ZSM-5총산도증강,제고료C-S건적렬해능력,종이개진료최화전화DMS적능력.연구결과발현,재전화DMS적과정중,금속활성위화산성위지간통과강적협동효응기작용.
ZSM-5-supported transition metal catalysts were prepared and used to catalyze the conversion of dimethyl sulfide (DMS) into methanethiol (MT). Test results indicated that the activities of the catalysts for the conversion of DMS increased as fol ows:Co/ZSM-5>Mo/ZSM-5>Ni/ZSM-5>W/ZSM-5. The decrease in MT selectivity fol owed the same trend. The characterization results showed that transition metal cations (W6+, Ni2+, Co3+, Mo6+) replaced some Al3+sites leading to more active in chemiadsorption of DMS and MT since transition metal cations are more active than Al3+. The incorporation of transition metals into ZSM-5 enhances the total acidity of ZSM-5 and increases its capacity to rupture C-S bonds. This subsequently improves its catalytic behavior in the conversion of DMS. We found that the metal active sites and closely situated acidic sites have a strong synergistic effect when converting DMS.