石河子大学学报(自然科学版)
石河子大學學報(自然科學版)
석하자대학학보(자연과학판)
JOURNAL OF SHIHEZI UNIVERSITY (NATURAL SCIENCE)
2014年
3期
360-365
,共6页
镧%固体超强酸%S2O82-/ZrO2-Al2O3%柠檬酸三丁酯
鑭%固體超彊痠%S2O82-/ZrO2-Al2O3%檸檬痠三丁酯
란%고체초강산%S2O82-/ZrO2-Al2O3%저몽산삼정지
lanthanum%solid super acid%S2O8/ZrO2-Al2O3%Tri-n-butyl citrate
柠檬酸三丁酯(TBC)是绿色环保无毒的增塑剂,其传统合成工艺采用浓硫酸作催化剂,设备腐蚀、三废问题严重,开发高效、绿色的替代催化剂是当前研究的重点。本文采用共沉淀-浸渍法向S2O82-/ZrO2-Al2O3催化剂中引入适量的La元素,制备出具有较高催化活性和稳定性的固体超强酸催化剂;以柠檬酸三丁酯的合成为探针反应评价催化剂的活性,并通过红外光谱、X射线衍射、NH3程序升温脱附,吡啶红外光谱等表征方法考察了La的添加对催化剂结构和性能的影响,结果表明:La的加入能够阻止催化剂中过硫酸根的分解,增强S和O之间的相互作用;少量的La不仅能增加催化剂的比表面积、酸强度和酸量,且能提高催化剂的活性和稳定性,当La的加载量为1%时,制得的催化剂活性最高,柠檬酸的转化率达到93.69%。这表明La的引入可提高固体超强酸催化剂的活性和稳定性,所制备的催化剂可用于传统催化剂浓硫酸的替代品,并有效降低设备的损耗,提高产品TBC的品质,优化TBC合成工艺,具有良好的经济价值。
檸檬痠三丁酯(TBC)是綠色環保無毒的增塑劑,其傳統閤成工藝採用濃硫痠作催化劑,設備腐蝕、三廢問題嚴重,開髮高效、綠色的替代催化劑是噹前研究的重點。本文採用共沉澱-浸漬法嚮S2O82-/ZrO2-Al2O3催化劑中引入適量的La元素,製備齣具有較高催化活性和穩定性的固體超彊痠催化劑;以檸檬痠三丁酯的閤成為探針反應評價催化劑的活性,併通過紅外光譜、X射線衍射、NH3程序升溫脫附,吡啶紅外光譜等錶徵方法攷察瞭La的添加對催化劑結構和性能的影響,結果錶明:La的加入能夠阻止催化劑中過硫痠根的分解,增彊S和O之間的相互作用;少量的La不僅能增加催化劑的比錶麵積、痠彊度和痠量,且能提高催化劑的活性和穩定性,噹La的加載量為1%時,製得的催化劑活性最高,檸檬痠的轉化率達到93.69%。這錶明La的引入可提高固體超彊痠催化劑的活性和穩定性,所製備的催化劑可用于傳統催化劑濃硫痠的替代品,併有效降低設備的損耗,提高產品TBC的品質,優化TBC閤成工藝,具有良好的經濟價值。
저몽산삼정지(TBC)시록색배보무독적증소제,기전통합성공예채용농류산작최화제,설비부식、삼폐문제엄중,개발고효、록색적체대최화제시당전연구적중점。본문채용공침정-침지법향S2O82-/ZrO2-Al2O3최화제중인입괄량적La원소,제비출구유교고최화활성화은정성적고체초강산최화제;이저몽산삼정지적합성위탐침반응평개최화제적활성,병통과홍외광보、X사선연사、NH3정서승온탈부,필정홍외광보등표정방법고찰료La적첨가대최화제결구화성능적영향,결과표명:La적가입능구조지최화제중과류산근적분해,증강S화O지간적상호작용;소량적La불부능증가최화제적비표면적、산강도화산량,차능제고최화제적활성화은정성,당La적가재량위1%시,제득적최화제활성최고,저몽산적전화솔체도93.69%。저표명La적인입가제고고체초강산최화제적활성화은정성,소제비적최화제가용우전통최화제농류산적체대품,병유효강저설비적손모,제고산품TBC적품질,우화TBC합성공예,구유량호적경제개치。
Tri-n-butyl citrate (TBC) as a green environmentally friendly and non-toxic plasticizer, and traditional synthesis process use the sulfuric acid as catalyst that corrosiveness to reactors and containers,and the serious problem of three wastes. Exploit of effective and green catalyst is the current research focus.In this work,highly active and stable solid superacid catalyst was prepared by simultaneously introducing appropriate amounts of La into a S2O82-/ZrO2-Al2O3 catalyst by precipitation and impregnation method.The catalytic performance for the synthesis of Tri-n-butyl citrate was investigated.The synthesized catalysts were fully characterized by means of FT-IR,XRD,NH3-TPD and FT-IR of adsorbed pyridine analysis methods.The experiments results show that the introduction of lanthanum inhibits the decomposition of sulfuric and strengthen the combination between S and O.A small number of La not only can increase the surface area and acid strength and the amount of acid sites of catalysts,but also can enhance the activity of catalyst.The catalyst loaded with 1wt% lanthanum samples exhibited higher activity for synthesis of Tri-n-butyl citrate and the conversion rate could reach 93.69%.This suggests that the addition of La improved activity and stability of solid superacid catalyst,and the resultant catalyst can be used to substitute for traditional sulfuric acid catalyst,which effectively reduce the wear and tear of equipment,improve the quality of the product TBC and optimize TBC synthesis process.In summary,the catalyst has the good economic value.