催化学报
催化學報
최화학보
CHINESE JOURNAL OF CATALYSIS
2015年
3期
380-388
,共9页
陈慧%赵杰%李少中%徐军%沈俭一
陳慧%趙傑%李少中%徐軍%瀋儉一
진혜%조걸%리소중%서군%침검일
镍%负载型催化剂%丙酮加氢%水的影响%吸附量热%红外光谱
鎳%負載型催化劑%丙酮加氫%水的影響%吸附量熱%紅外光譜
얼%부재형최화제%병동가경%수적영향%흡부량열%홍외광보
Nickel%Supported catalyst%Hydrogenation of acetone%Effect of water%Microcalorimetric adsorption%Fourier transform infrared spectroscopy
研究了H2O对Ni/MgAlO催化剂上丙酮加氢为异丙醇的催化反应的影响。结果发现,在丙酮中添加少量H2O可提高丙酮转化率,但超过5%的H2O量则会显著降低催化剂活性。吸附量热结果表明,催化剂表面吸附少量H2O会明显降低异丙醇的吸附热,但对丙酮吸附热的影响较小,这也许是反应体系中少量的H2O能促进丙酮加氢活性的原因之一。当催化剂表面吸附较多H2O后,丙酮、异丙醇和H2的吸附热都降低了,因此反而抑制了丙酮的加氢反应。此外,红外光谱结果表明,预吸附水抑制了催化剂表面异丙醇脱氢生成丙酮,并抑制吸附的丙酮在表面生成烯醇盐或异丙叉丙酮等物种,这也许是少量水能促进丙酮加氢生成异丙醇的另一个重要原因。
研究瞭H2O對Ni/MgAlO催化劑上丙酮加氫為異丙醇的催化反應的影響。結果髮現,在丙酮中添加少量H2O可提高丙酮轉化率,但超過5%的H2O量則會顯著降低催化劑活性。吸附量熱結果錶明,催化劑錶麵吸附少量H2O會明顯降低異丙醇的吸附熱,但對丙酮吸附熱的影響較小,這也許是反應體繫中少量的H2O能促進丙酮加氫活性的原因之一。噹催化劑錶麵吸附較多H2O後,丙酮、異丙醇和H2的吸附熱都降低瞭,因此反而抑製瞭丙酮的加氫反應。此外,紅外光譜結果錶明,預吸附水抑製瞭催化劑錶麵異丙醇脫氫生成丙酮,併抑製吸附的丙酮在錶麵生成烯醇鹽或異丙扠丙酮等物種,這也許是少量水能促進丙酮加氫生成異丙醇的另一箇重要原因。
연구료H2O대Ni/MgAlO최화제상병동가경위이병순적최화반응적영향。결과발현,재병동중첨가소량H2O가제고병동전화솔,단초과5%적H2O량칙회현저강저최화제활성。흡부량열결과표명,최화제표면흡부소량H2O회명현강저이병순적흡부열,단대병동흡부열적영향교소,저야허시반응체계중소량적H2O능촉진병동가경활성적원인지일。당최화제표면흡부교다H2O후,병동、이병순화H2적흡부열도강저료,인차반이억제료병동적가경반응。차외,홍외광보결과표명,예흡부수억제료최화제표면이병순탈경생성병동,병억제흡부적병동재표면생성희순염혹이병차병동등물충,저야허시소량수능촉진병동가경생성이병순적령일개중요원인。
The effect of water on the hydrogenation of acetone to isopropanol (IPA) on the Ni/MgAlO catalyst was studied. It was found that small amount of water added in the acetone promoted the conversion of acetone to IPA, while more H2O added (>5%) significantly decreased the conversion of acetone. Microcalorimetric adsorption results showed that the presence of small amount of pre‐adsorbed water (4%coverage) enhanced the adsorption of acetone while inhibited the adsorption of IPA on Ni, which might be the important reasons for the promotion effect of some water on the hydrogena‐tion of acetone to IPA. On the other hand, the heats for the adsorption of H2, acetone and IPA on the Ni/MgAlO were significantly decreased when more water was pre‐adsorbed, which might explain the inhibition effect of more water on the hydrogenation of acetone. The results of infrared spec‐troscopy revealed that the presence of water suppressed the dehydrogenation of adsorbed IPA to acetone and the formation of enolate and mesityl oxide species from adsorbed acetone, which might be the other reasons for the positive effect of water on the hydrogenation of acetone to IPA.