催化学报
催化學報
최화학보
CHINESE JOURNAL OF CATALYSIS
2015年
5期
721-727
,共7页
李念哲%高远%张欣欣%玉占君%石雷%孙琪
李唸哲%高遠%張訢訢%玉佔君%石雷%孫琪
리념철%고원%장흔흔%옥점군%석뢰%손기
苯乙烯%双氧水%对甲苯磺酸%活性炭%氧化
苯乙烯%雙氧水%對甲苯磺痠%活性炭%氧化
분을희%쌍양수%대갑분광산%활성탄%양화
Styrene%Hydrogen peroxide%p-Toluenesulfonic acid%Activated carbon%Oxidation
以双氧水为氧化剂,研究了对甲苯磺酸和活性炭体系选择氧化苯乙烯生成苯甲醛反应性能。考察了反应时间、温度、催化剂用量、苯乙烯和双氧水摩尔比等对苯乙烯选择氧化性能的影响。结果表明,对甲苯磺酸和活性炭的用量和用量比是一个重要因素,但对甲苯磺酸的酸性对氧化反应活性影响不大。对甲苯磺酸和双氧水相互作用,经非自由基过程氧化苯乙烯。通过分解双氧水产生氢氧自由基,活性炭显著提高对甲苯磺酸和双氧水体系氧化苯乙烯活性。在惰性或还原气氛中高温处理活性炭能降低其表面含氧基团数量,增加碱性,有效分解双氧水,产生相对较多的OH自由基。与未处理的活性炭相比,高温处理的活性炭进一步提高了对甲苯磺酸和双氧水体系氧化苯乙烯活性,但降低了苯甲醛选择性。经磺化,在活性炭表面引入的–SO3H基团比含氧基团(–OH,–COOH)更有效与双氧水作用氧化苯乙烯。
以雙氧水為氧化劑,研究瞭對甲苯磺痠和活性炭體繫選擇氧化苯乙烯生成苯甲醛反應性能。攷察瞭反應時間、溫度、催化劑用量、苯乙烯和雙氧水摩爾比等對苯乙烯選擇氧化性能的影響。結果錶明,對甲苯磺痠和活性炭的用量和用量比是一箇重要因素,但對甲苯磺痠的痠性對氧化反應活性影響不大。對甲苯磺痠和雙氧水相互作用,經非自由基過程氧化苯乙烯。通過分解雙氧水產生氫氧自由基,活性炭顯著提高對甲苯磺痠和雙氧水體繫氧化苯乙烯活性。在惰性或還原氣氛中高溫處理活性炭能降低其錶麵含氧基糰數量,增加堿性,有效分解雙氧水,產生相對較多的OH自由基。與未處理的活性炭相比,高溫處理的活性炭進一步提高瞭對甲苯磺痠和雙氧水體繫氧化苯乙烯活性,但降低瞭苯甲醛選擇性。經磺化,在活性炭錶麵引入的–SO3H基糰比含氧基糰(–OH,–COOH)更有效與雙氧水作用氧化苯乙烯。
이쌍양수위양화제,연구료대갑분광산화활성탄체계선택양화분을희생성분갑철반응성능。고찰료반응시간、온도、최화제용량、분을희화쌍양수마이비등대분을희선택양화성능적영향。결과표명,대갑분광산화활성탄적용량화용량비시일개중요인소,단대갑분광산적산성대양화반응활성영향불대。대갑분광산화쌍양수상호작용,경비자유기과정양화분을희。통과분해쌍양수산생경양자유기,활성탄현저제고대갑분광산화쌍양수체계양화분을희활성。재타성혹환원기분중고온처리활성탄능강저기표면함양기단수량,증가감성,유효분해쌍양수,산생상대교다적OH자유기。여미처리적활성탄상비,고온처리적활성탄진일보제고료대갑분광산화쌍양수체계양화분을희활성,단강저료분갑철선택성。경광화,재활성탄표면인입적–SO3H기단비함양기단(–OH,–COOH)경유효여쌍양수작용양화분을희。
The selective oxidation of styrene to benzaldehyde catalyzed byp-toluenesulfonic acid (p-TsOH) in the presence of activated carbon (AC) was investigated with H2O2 as the oxidant. The reaction pa-rameters of reaction time, temperature, catalyst mass, and styrene/H2O2 molar ratios were evalu-ated. A strong promoting effect of AC on thep-TsOH/H2O2 system was observed. The appropriate ratio and amounts of AC andp-TsOH were an important factor. The acidity ofp-TsOH does not play a significant role.p-TsOH reacted with H2O2 by a non-radical process to oxidize styrene. The func-tion of the AC was to activate H2O2and to help thep-TsOH/H2O2 system in styrene oxidation. The reduction of oxygen containing groups (–OH, –COOH) on AC by a high temperature treatment or introduction of –SO3H groups onto AC affected the styrene conversion. The –SO3H groups were more effective than the oxygen-containing groups on the AC in promoting styrene oxidation.