佳木斯大学学报(自然科学版)
佳木斯大學學報(自然科學版)
가목사대학학보(자연과학판)
JOURNAL OF JIAMUSI UNIVERSITY (NATURAL SCIENCE EDITION)
2014年
3期
471-474
,共4页
徐锋%贾韶洋%朱丽华%胡成秋%陈文胜%李定启%王伟
徐鋒%賈韶洋%硃麗華%鬍成鞦%陳文勝%李定啟%王偉
서봉%가소양%주려화%호성추%진문성%리정계%왕위
Pd/C%醋酸%瓦斯%甲醇%机理%选择氧化
Pd/C%醋痠%瓦斯%甲醇%機理%選擇氧化
Pd/C%작산%와사%갑순%궤리%선택양화
Pd/C%acetic acid%mine gas%methanol%mechanism%selective oxidation
为有效利用瓦斯资源,研究了瓦斯选择氧化制甲醇的反应条件及机理.以PdCl 2为前驱体,采用浸渍法制备了Pd/C催化剂,进而对醋酸水溶液中Pd/C催化瓦斯选择氧化制甲醇的反应条件进行了实验研究,结果表明,目标产物甲醇生成量与催化剂添加量、对苯醌用量、溶剂中CH3 COOH与H2 O的混合比例、反应温度和反应时间正相关.采用3%Pd/C为催化剂时,在3%Pd/C添加量2g、对苯醌用量1000μmol、CH3 COOH与H2 O体积比4:1、反应温度130℃、反应时间3h条件下,甲醇的生成量为1960μmol.此外,利用瓦斯选择氧化实验和XRD谱图表征技术研究了Pd/C催化剂循环使用对瓦斯氧化制甲醇的影响.分析实验结果,认为Pd/C在醋酸溶液中催化瓦斯选择氧化制甲醇反应,既遵循亲电取代机理,又遵循活性氧物种氧化机理.
為有效利用瓦斯資源,研究瞭瓦斯選擇氧化製甲醇的反應條件及機理.以PdCl 2為前驅體,採用浸漬法製備瞭Pd/C催化劑,進而對醋痠水溶液中Pd/C催化瓦斯選擇氧化製甲醇的反應條件進行瞭實驗研究,結果錶明,目標產物甲醇生成量與催化劑添加量、對苯醌用量、溶劑中CH3 COOH與H2 O的混閤比例、反應溫度和反應時間正相關.採用3%Pd/C為催化劑時,在3%Pd/C添加量2g、對苯醌用量1000μmol、CH3 COOH與H2 O體積比4:1、反應溫度130℃、反應時間3h條件下,甲醇的生成量為1960μmol.此外,利用瓦斯選擇氧化實驗和XRD譜圖錶徵技術研究瞭Pd/C催化劑循環使用對瓦斯氧化製甲醇的影響.分析實驗結果,認為Pd/C在醋痠溶液中催化瓦斯選擇氧化製甲醇反應,既遵循親電取代機理,又遵循活性氧物種氧化機理.
위유효이용와사자원,연구료와사선택양화제갑순적반응조건급궤리.이PdCl 2위전구체,채용침지법제비료Pd/C최화제,진이대작산수용액중Pd/C최화와사선택양화제갑순적반응조건진행료실험연구,결과표명,목표산물갑순생성량여최화제첨가량、대분곤용량、용제중CH3 COOH여H2 O적혼합비례、반응온도화반응시간정상관.채용3%Pd/C위최화제시,재3%Pd/C첨가량2g、대분곤용량1000μmol、CH3 COOH여H2 O체적비4:1、반응온도130℃、반응시간3h조건하,갑순적생성량위1960μmol.차외,이용와사선택양화실험화XRD보도표정기술연구료Pd/C최화제순배사용대와사양화제갑순적영향.분석실험결과,인위Pd/C재작산용액중최화와사선택양화제갑순반응,기준순친전취대궤리,우준순활성양물충양화궤리.
This paper referred to the catalyst prepared by taking PdCl 2 as the precursor , and investigated the reaction conditions of the selective oxidation of mine gas to methanol in the aqueous solution of acetic acid o -ver Pd/C catalyst.The results show that the production of the target product , i.e.methanol is positively related to the addition of the catalyst , the addition of p-benzoquinone , the mixing proportion of CH 3 COOH and H2 O in the solvent , the temperature and time of reaction .In case of the use of 3%Pd/C as the catalyst , the production of methanol is 1960μmol in the condition that the addition of the 3%Pd/C is 2g, the addition of p-benzoqui-none is 1000μmol, the volume ratio between CH 3 COOH and H2 O is 4:1, the temperature is 130℃, and the re-action time is 3h.Moreover, effect of recycled Pd/C catalyst on selective oxidation of mine gas to methanol is studied .The methanol synthesized by catalyzing the selective oxidation of gas in the acetic acid solution through Pd/C may be the result for the joint action of electrophilic substitution reaction and oxidation of reactive oxygen species .