催化学报
催化學報
최화학보
CHINESE JOURNAL OF CATALYSIS
2014年
3期
302-309
,共8页
张兴华%张琦%陈伦刚%徐莹%王铁军%马隆龙
張興華%張琦%陳倫剛%徐瑩%王鐵軍%馬隆龍
장흥화%장기%진륜강%서형%왕철군%마륭룡
镍%氧化硅%氧化锆%焙烧温度%愈创木酚%加氢脱氧%环己烷
鎳%氧化硅%氧化鋯%焙燒溫度%愈創木酚%加氫脫氧%環己烷
얼%양화규%양화고%배소온도%유창목분%가경탈양%배기완
Nickel%Silica%Zirconia%Calcination temperature%Guaiacol%Hydrodeoxygenation%Cyclohexane
采用化学沉淀法合成了SiO2-ZrO2复合氧化物载体,并以浸渍法制备了Ni/SiO2-ZrO2双功能催化剂,考察了焙烧温度对催化剂结构及其催化愈创木酚加氢脱氧制环己烷性能的影响.结果表明,经500°C焙烧催化剂的加氢脱氧活性最高,在Ni金属中心和SiO2-ZrO2载体材料的协同作用下,愈创木酚转化率为100%,环己烷选择性为96.8%.对催化剂进行N2物理吸附、H2化学吸附、X射线衍射分析、H2程序升温还原、NH3程序升温脱附与Raman光谱等表征后发现,合成的SiO2-ZrO2为无定形的酸碱两性氧化物;经500°C焙烧的催化剂样品的有效比表面积和孔体积均明显增大,表面酸量最多,硝酸镍分解成小颗粒的NiO较易被H2还原,这些特性是该催化剂样品具有高效加氢脱氧活性的原因.
採用化學沉澱法閤成瞭SiO2-ZrO2複閤氧化物載體,併以浸漬法製備瞭Ni/SiO2-ZrO2雙功能催化劑,攷察瞭焙燒溫度對催化劑結構及其催化愈創木酚加氫脫氧製環己烷性能的影響.結果錶明,經500°C焙燒催化劑的加氫脫氧活性最高,在Ni金屬中心和SiO2-ZrO2載體材料的協同作用下,愈創木酚轉化率為100%,環己烷選擇性為96.8%.對催化劑進行N2物理吸附、H2化學吸附、X射線衍射分析、H2程序升溫還原、NH3程序升溫脫附與Raman光譜等錶徵後髮現,閤成的SiO2-ZrO2為無定形的痠堿兩性氧化物;經500°C焙燒的催化劑樣品的有效比錶麵積和孔體積均明顯增大,錶麵痠量最多,硝痠鎳分解成小顆粒的NiO較易被H2還原,這些特性是該催化劑樣品具有高效加氫脫氧活性的原因.
채용화학침정법합성료SiO2-ZrO2복합양화물재체,병이침지법제비료Ni/SiO2-ZrO2쌍공능최화제,고찰료배소온도대최화제결구급기최화유창목분가경탈양제배기완성능적영향.결과표명,경500°C배소최화제적가경탈양활성최고,재Ni금속중심화SiO2-ZrO2재체재료적협동작용하,유창목분전화솔위100%,배기완선택성위96.8%.대최화제진행N2물리흡부、H2화학흡부、X사선연사분석、H2정서승온환원、NH3정서승온탈부여Raman광보등표정후발현,합성적SiO2-ZrO2위무정형적산감량성양화물;경500°C배소적최화제양품적유효비표면적화공체적균명현증대,표면산량최다,초산얼분해성소과립적NiO교역피H2환원,저사특성시해최화제양품구유고효가경탈양활성적원인.
SiO2-ZrO2 composites were synthesized by chemical precipitation and used to prepare a series of bifunctional Ni/SiO2-ZrO2 catalysts by impregnation. The effect of calcination temperature on the catalyst structure and its catalysis of the hydrodeoxygenation of guaiacol was investigated. Guaiacol was converted to cyclohexane by a synergism between the metal center and solid acid support. The catalyst calcined at 500 °C gave a maximum 100% guaiacol conversion and 96.8% selectivity for cyclohexane. The catalyst samples were characterized by N2 adsorption, H2 chemisorption, X-ray diffraction, H2 temperature-programmed reduction, NH3 temperature-programmed desorption, and Raman spectroscopy. The synthesized SiO2-ZrO2 was an amorphous oxide. The Ni/SiO2-ZrO2 catalyst calcined at 500 °C has more acidity, smaller NiO particles, and larger BET surface area and pore volume, which gave it the best catalytic performance.