CN105688803A - 衍生自有机物质的挥发性有机化合物的吸附 - Google Patents
衍生自有机物质的挥发性有机化合物的吸附 Download PDFInfo
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- CN105688803A CN105688803A CN201610080998.XA CN201610080998A CN105688803A CN 105688803 A CN105688803 A CN 105688803A CN 201610080998 A CN201610080998 A CN 201610080998A CN 105688803 A CN105688803 A CN 105688803A
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Abstract
本发明涉及掺杂钯的ZSM-5用以吸附衍生自有机物质的挥发性有机化合物(VOC)的用途,其中所述ZSM-5的Si:Al比小于或等于100:1,并且其中所述掺杂钯的ZSM-5用在包含小于10vol%氧气的环境中。
Description
本申请是基于申请号为201080029809.7、申请日为2010年7月2日、发明名称为“衍生自有机物质的挥发性有机化合物的吸附”的中国专利申请的分案申请。
本发明涉及在含有低氧气或无氧气的环境中吸附衍生自有机物质的挥发性有机化合物(VOC)。更具体地,有机物质可以是易腐烂有机物品,例如食品。
新鲜产品的受控气氛贮藏利用高的CO2含量和减少的氧气来提高产品的贮存期。调节气氛包装通过降低与空气相比的气氛中的氧气的量(逼近零)用以提高食品的寿命和/或品质。新鲜产品趋向于在平衡调节气氛下进行包装,所述气氛使用高的CO2含量和减少的氧气含量并且允许降低的呼吸速率。
VOC包括衍生自有机物质的一系列化合物。衍生自有机物质的VOC的一个实例是乙烯(导致熟化的植物激素),而另一个实例是三甲胺(一般由鱼在其腐烂时放出的气体)。
去除衍生自有机物质的VOC对于各种应用而言具有重要意义。乙烯的吸附可防止水果和蔬菜中发生不期望的熟化和变软、褪色、掉叶和发芽,还已知防止其它食品和园艺产品不早熟腐烂,并且可有助于消除令人不愉快的气味。
使用Al2O3上的Pt或KMnO4采用各种方法来氧化或燃烧VOC。然而,虽然这些系统对于VOC的去除是有效的,但是它们具有伴随它们的使用的缺点。Al2O3上的Pt通过在升高的温度下催化燃烧乙烯发挥作用,因此Al2O3上的Pt需要在与VOC来源分开的加热的单元中使用(参见例如GB2163637A和US4,331,693)。KMnO4似乎不能有效地从湿环境除去VOC。因为有机物质,例如食品,不可能受到加热而不改变,并且固有地渗出水分,所以这类系统都不适合用于除去衍生自有机物质的VOC。
用于除去VOC的其它方法适合用在较低的温度下;这些包括使用高表面积载体,通常与促进剂结合,用以吸附VOC。例如,JP2-261341涉及吸附来自冷藏隔室的乙烯,JP2-233381涉及乙烯吸附膜,和JP2000-004783涉及用于冰箱的组合的乙烯吸附剂、除臭剂和抗细菌产品。任何这些出版物中没有公开特殊载体材料,而是宣称活性炭和金属氧化物通常适合用作载体。GB2252968A涉及包含与沸石组合的海泡石,和任选选自铂族金属、铁族金属、第I族金属、第VII金属和稀土金属的金属的吸附剂。描述于GB‘968中的用于本发明的最优选的沸石是硅沸石,这是因为它们的氧化铝含量几乎为零。
WO2007/052074涉及使用掺杂钯的ZSM-5来吸附衍生自有机物质的VOC。然而,WO2007/052074没有述及在包含低气态氧或无气态氧的环境中使用掺杂钯的ZSM-5。
根据本发明的第一方面,提供了掺杂钯的ZSM-5用以吸附衍生自有机物质的VOC的用途,其中ZSM-5的Si:Al比小于或等于100:1,并且其中掺杂钯的ZSM-5用在包含小于10vol%氧气的环境中。任选地ZSM-5的Si:Al比为22:1-28:1。
至少部分所吸附的VOC在吸附到掺杂ZSM-5上之后可以转化为次生化合物。
在一个实施方案中,有机物质包括易腐烂有机物品,例如食品和园艺产品。食品可以包含水果和/或蔬菜。园艺产品可以包含植物和/或切花。
在另一个实施方案中,有机物质包含废弃物。这种废弃物可以包括厨余垃圾例如废弃食品,其产生令人不愉快的气味并同时分解。
衍生出VOC的有机物质可以容纳在贮藏容器或包装中,使得掺杂的ZSM-5具有封闭或半封闭的环境,在该环境内吸附VOC。在易腐烂有机物品的情形中,贮藏容器或包装有可能是在其内容纳物品的容器或包装,例如运送时用于贮藏物品的箱子(crate)或购买前展示时将物品保存于其内的包装。在另一个实施方案中,将掺杂的ZSM-5纳入贮藏容器或包装本身中或者所述贮藏容器或包装本身的一部分中。在其它实施方案中,将掺杂的ZSM-5纳入标签(label)中,所述标签包含用于插入和保持在贮藏容器或包装内的基材(substrate)。
如果易腐烂有机物品包含食品,则可以将掺杂的ZSM-5以防止与食品直接接触的方式例如在透气阻挡层之后进行包装。透气阻挡层可以形成包封粉末状掺杂ZSM-5的袋(sachet)或标签的一部分,或者可将透气层附在包含掺杂的ZSM-5的墨层顶部上。可通过印刷、浇注、辊压施加、刷涂、喷涂等技术将墨固定到贮藏容器或包装的内表面。另外,由于掺杂的ZSM-5的吸附能力对水的存在适度敏感,掺杂的ZSM-5可以用吸水性材料例如硅胶(silicagel)进行包装。
然而,如果VOC的来源是废弃物,则贮藏容器或包装可以是废弃物贮器。
一般地,掺杂的ZSM-5可以是粒料并且可以松散地进行包装,例如包装在袋内(参见上文)。或者,所述粒料可以与另一物体结合,例如通过纳入贮藏容器中、纳入包装材料(例如塑料,如PET)中、纳入墨中(参见上文),或者简单地涂覆到另一物体例如陶瓷或金属独石(如用作催化剂载体的那些)之上或之内。还可以使用其它形式的低压降基材,例如一般用作催化剂载体的那些。在另一个实施方案中,掺杂的ZSM-5是挤出物、丸粒、片剂、颗粒(grain)或粒料的形式。ZSM-5可以在成形为这样的挤出物、丸粒、片剂、颗粒或粒料之前或之后进行掺杂。
可以在适当情况中采用其它使用本发明的其它方法。
与本发明有关的一个优点是可以在相对低的温度例如-10℃至50℃,更一般地0℃至40℃下吸附VOC。例如,温度范围可以为约0℃至约35℃或约0℃至约30℃。这使掺杂的ZSM-5能够用于在其中一般遇到有机物质的环境中,例如冰箱中或在环境温度下,不需要使用复杂的加热和气体再循环设备。然而,在具体应用允许使用加热和气体再循环设备(例如气体调节系统)时,掺杂的ZSM-5还可以在提高的温度例如高于60℃下进行操作。
在一个实施方案中,VOC包含乙烯。乙烯是植物释放的可导致植物枯萎和水果成熟的气体激素。植物产生的VOC的去除可延迟这些过程从而使食品和园艺产品能够在运送和/或贮藏中保存较久而没有加速腐烂。因此,本发明的具体应用是生产、运输(ship)、出口和购买食品和园艺产品的行业。初步试验暗示,与现有技术方法不同,根据本发明的吸附剂用途会使颓化后(post-climacteric)水果的贮存期能够延长(TerryL,IIkenhansT,PoulstonS,RowsellE和SmithAWJ,PostharvestBiologyandTechnology45(2007)214-220)。也就是,即使在开始颓化呼吸上升之后,使用掺杂钯的ZSM-5吸附乙烯也可以防止水果不进一步熟化(或至少减缓熟化速率)。
在另一个实施方案中,VOC包含甲醛和/或乙酸。甲醛和乙酸是经常在家中遇到的气味难闻的化学品。甲醛可以从压制粘合的木材制品例如胶合板释放,也在染料、织物、塑料、纸制品、肥料和化妆品中遇到。乙酸可以从厨余废物和动物废物释放。因此,本发明的一个潜在应用是从家庭环境除去难闻气味。
另一个关注点是,虽然一旦将掺杂钯的ZSM-5暴露于水时,它们的活性有一些丧失,但是它们仍能够在“湿”时有效地发挥作用。因为食品和园艺产品通常贮藏在潮湿环境中,这种特征对于相关行业也是有利的。
制造掺杂钯的ZSM-5的方法对熟练化学工作者而言是已知的,并且包括使用各种钯盐,例如Pd(NO3)2、Pd(OAc)2、PdCl2、草酸钯、(碳酸氢四氨合钯)、(氢氧化四氨合钯)和(乙酸四氨合钯)。一般地,ZSM-5可在用至少一种钯盐浸渍之后煅烧,然而,对于一些应用,这可能并非必须。煅烧的掺杂钯的ZSM-5的样品将包含至少部分氧化的钯。
钯本身可以基于ZSM-5总重量计占0.1wt%-10.0wt%,任选基于ZSM-5总重量计占0.5wt%-5.0wt%。
掺杂的ZSM-5可以合宜地用于受控气氛环境或调节气氛环境。在一个实施方案中,这些环境中的氧含量以≥0.5vol%至<10vol%存在。例如,氧含量可以为约1vol%、约2vol%、约3vol%、约4vol%、约5vol%、约6vol%、约7vol%、约8vol%或约9vol%。在另一个实施方案中,氧气含量为基本上0vol%。气体组合物的余量可以包含惰性气体(例如氮气),任选二氧化碳和/或任选一氧化碳。
在一个实施方案中,掺杂的ZSM-5对于将VOC吸附至小于或等于0.10ppm的水平,任选吸附至小于或等于0.05ppm的水平是有效将。在另一个实施方案中,掺杂的ZSM-5有效吸附基本上所有VOC,即没有残留可检测的量的VOC。
本发明的另一个优点是,掺杂的ZSM-5可以长时期地例如几天连续用于VOC去除(实际时间取决于其中使用它的环境)。此外,在使用后可以在空气中将ZSM-5加热到250℃并持续30分钟以释放ZSM-5上吸附的VOC和存在的任何次生化合物,因此使掺杂钯的ZSM-5再生用于另外使用。这使掺杂钯的ZSM-5能够长时间段地使用,然后从VOC源取出,进行再生和再用。因为再生过程既不冗长又不昂贵,这意味着掺杂的ZSM-5是用于除去VOC的成本有效的产品。应值得注意的是,相比而言,KMnO4的再生是不可能的,这是因为该物质在加热时分解为K2O和锰氧化物。
为了确定掺杂的ZSM-5已达到其VOC吸附容量并因此需要再生时的时间,可以纳入VOC指示剂用于与掺杂ZSM-5一起使用。
合适的指示剂包括公开于专利申请JP60-202252中的钯基乙烯指示剂。
本发明的实施方案包括:
1.掺杂钯的ZSM-5用以吸附衍生自有机物质的挥发性有机化合物(VOC)的用途,其中所述ZSM-5的Si:Al比小于或等于100:1,并且其中所述掺杂钯的ZSM-5用在包含小于10vol%氧气的环境中。
2.根据实施方案1的用途,其中所述ZSM-5的Si:Al比为22:1-28:1。
3.根据实施方案1或2的用途,其中所述有机物质包括易腐烂有机物品。
4.根据实施方案3的用途,其中所述易腐烂有机物品包含食品。
5.根据实施方案4的用途,其中所述食品包含水果和/或蔬菜。
6.根据实施方案1或2的用途,其中所述易腐烂有机物品包含园艺产品。
7.根据实施方案6的用途,其中所述园艺产品包含植物和/或切花。
8.根据实施方案1或2的用途,其中所述有机物质包含废弃物。
9.根据前述实施方案中任一项的用途,其中所述有机物质容纳在贮藏容器或包装中。
10.根据实施方案9的用途,其中将所述掺杂钯的ZSM-5纳入贮藏容器或包装中或者所述贮藏容器或包装的一部分中。
11.根据实施方案9的用途,其中将所述掺杂钯的ZSM-5纳入标签中,所述标签包含用于插入和保持在贮藏容器或包装内的基材。
12.根据实施方案9、10或11的用途,其中所述贮藏容器或包装是废弃物贮器。
13.根据前述实施方案中任一项的用途,其中在-10℃至50℃的温度下吸附VOC。
14.根据实施方案13的用途,其中在0℃至约40℃,优选0℃至30℃的温度下吸附VOC。
15.根据前述实施方案中任一项的用途,其中VOC包含乙烯。
16.根据前述实施方案中任一项的用途,其中VOC包含甲醛和/或乙酸。
17.根据前述实施方案中任一项的用途,其中钯基于掺杂ZSM-5的总重量计占0.1wt%-10.0wt%。
18.根据实施方案17的用途,其中钯基于掺杂ZSM-5的总重量计占0.5wt%-5.0wt%。
19.根据前述实施方案中任一项的用途,其中所述环境是受控气氛环境或调节气氛环境。
20.根据前述实施方案中任一项的用途,其中氧气以≥0.5vol%且<10vol%存在。
21.根据前述实施方案中任一项的用途,其中将VOC吸附至小于或等于0.10ppm的水平。
22.根据实施方案24的用途,其中将VOC吸附至小于或等于0.05ppm的水平。
23.根据前述实施方案中任一项的用途,其中在空气中将掺杂钯的ZSM-5加热到250℃并持续30分钟以释放该掺杂钯的ZSM-5上吸附的VOC和存在的任何次生化合物,因此使掺杂钯的ZSM-5再生用于另外使用。
24.根据前述实施方案中任一项的用途,其中所述掺杂钯的ZSM-5与VOC指示剂一起使用。
25.根据前述实施方案中任一项的用途,其中所述掺杂钯的ZSM-5是标签、袋或墨的形式,或者被涂覆到催化剂载体之上或之中,或者是挤出物、丸粒、片剂、颗粒或粒料的形式,或者被纳入包装材料中。
为了可以更充分地理解本发明,以仅仅描述方式并且参考附图提供以下非限制性实施例,其中:
图1是显示掺杂有钯的ZSM-5在包含约8.4vol%氧气的环境中的乙烯吸附随时间的坐标图。
实施例1
掺杂载体的制备
使用始润浸渍法制备掺杂载体(也称作吸附剂)。通常将20g载体(例如氢型沸石)用钯的硝酸盐或氯化物盐浸渍,然后在110℃下干燥,之后在空气中于500℃下煅烧2小时。
实施例2
乙烯吸附测量
在活塞流反应器中于21℃下用0.1g颗粒尺寸为250-355μm的掺杂载体以及流速为50ml/min的包含变化浓度的O2、200ppmC2H4、~80%相对湿度和余量氮气的气体进行测量。下面给出了该实验的结果:
O2浓度/vol% | 乙烯吸附容量/μl.g-1 |
10 | 3500 |
4 | 3600 |
2 | 3800 |
1 | 3700 |
0 | 6050 |
实施例3
乙烯吸附测量
在21℃下用0.1g颗粒尺寸为250-355μm的掺杂载体进行测量。将1升广口瓶(jar)部分抽空并然后用在氮气中的500ppm乙烯进行填充,其与剩余空气混合,使得初始O2浓度为8.4vol%。
图1描述了在约12小时的时段内掺杂Pd的载体吸附基本上所有乙烯。
Claims (29)
1.掺杂钯的氢-ZSM-5用以吸附衍生自有机物质的挥发性有机化合物(VOC)的用途,其中所述氢-ZSM-5的Si:Al比小于或等于100:1,并且其中所述掺杂钯的氢-ZSM-5用在包含以下的环境中:0vol%、1vol%、2vol%、3vol%、4vol%、5vol%、6vol%、7vol%、8vol%或9vol%的氧气,并且余量包含氮气、任选的二氧化碳和/或一氧化碳。
2.根据权利要求1所述的用途,其中所述氢-ZSM-5的Si:Al比为22:1-28:1。
3.根据权利要求1所述的用途,其中所述有机物质由易腐烂有机物品组成。
4.根据权利要求3所述的用途,其中所述易腐烂有机物品包括食品。
5.根据权利要求4所述的用途,其中所述食品包括水果和/或蔬菜。
6.根据权利要求1所述的用途,其中所述易腐烂有机物品包括园艺产品。
7.根据权利要求6所述的用途,其中所述园艺产品包括植物和/或切花。
8.根据权利要求1所述的用途,其中所述有机物质包括废弃物。
9.根据权利要求1所述的用途,其中所述有机物质容纳在贮藏容器或包装中。
10.根据权利要求9所述的用途,其中将所述掺杂钯的氢-ZSM-5纳入贮藏容器或包装中或者所述贮藏容器或包装的一部分中。
11.根据权利要求9所述的用途,其中将所述掺杂钯的氢-ZSM-5纳入标签中,所述标签包含用于插入和保持在贮藏容器或包装内的基材。
12.根据权利要求9、10或11所述的用途,其中所述贮藏容器或包装是废弃物贮器。
13.根据权利要求1所述的用途,其中在-10℃至50℃的温度下吸附VOC。
14.根据权利要求13所述的用途,其中在0℃至约40℃,优选0℃至30℃的温度下吸附VOC。
15.根据权利要求1所述的用途,其中VOC包括乙烯。
16.根据权利要求1所述的用途,其中VOC包括甲醛和/或乙酸。
17.根据权利要求1所述的用途,其中钯基于掺杂的氢-ZSM-5的总重量计占0.1wt%-10.0wt%。
18.根据权利要求17所述的用途,其中钯基于掺杂的氢-ZSM-5的总重量计占0.5wt%-5.0wt%。
19.根据权利要求1所述的用途,其中所述环境是受控气氛环境或调节气氛环境。
20.根据权利要求1所述的用途,其中氧气以≥0.5vol%至9vol%存在。
21.根据权利要求1所述的用途,其中氧气以≥0.5vol%至8vol%存在。
22.根据权利要求1所述的用途,其中氧气以≥0.5vol%至7vol%存在。
23.根据权利要求1所述的用途,其中氧气以≥0.5vol%至6vol%存在。
24.根据权利要求1所述的用途,其中氧气以≥0.5vol%至5vol%存在。
25.根据权利要求1所述的用途,其中将VOC吸附至小于或等于0.10ppm的水平。
26.根据权利要求25所述的用途,其中将VOC吸附至小于或等于0.05ppm的水平。
27.根据权利要求1所述的用途,其中在空气中将所述掺杂钯的氢-ZSM-5加热到250℃并持续30分钟以释放所述掺杂钯的氢-ZSM-5上吸附的VOC和存在的任何次生化合物,因此使所述掺杂钯的氢-ZSM-5再生以进一步使用。
28.根据权利要求1所述的用途,其中所述掺杂钯的氢-ZSM-5与VOC指示剂一起使用。
29.根据权利要求1所述的用途,其中所述掺杂钯的氢-ZSM-5是标签、袋或墨的形式,或者被涂覆到催化剂载体之上或之中,或者是挤出物、丸粒、片剂、颗粒或粒料的形式,或者被纳入包装材料中。
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