CN1980575B - 含thp盐的增效杀生物组合物 - Google Patents

含thp盐的增效杀生物组合物 Download PDF

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CN1980575B
CN1980575B CN2005800039265A CN200580003926A CN1980575B CN 1980575 B CN1980575 B CN 1980575B CN 2005800039265 A CN2005800039265 A CN 2005800039265A CN 200580003926 A CN200580003926 A CN 200580003926A CN 1980575 B CN1980575 B CN 1980575B
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R·E·塔尔博特
C·R·琼斯
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Abstract

本发明涉及一种包含THP盐和生物渗透剂的增效组合物，其中生物渗透剂包括不饱和羧酸的聚合物或不饱和羧酸与磺酸的共聚物，所述聚合物或共聚物由单-或二膦酸化的不饱和羧酸基团封端或具有引入聚合物骨架的这类单体。该组合物对提高THP盐对浮游(自由游动)和固着的(附着的)细菌杀生物效力具有增效作用，还对提高THP盐溶解硫化铁锈的效力有增效作用。

Description

含THP盐的增效杀生物组合物
本发明涉及增效杀生物组合物或溶解金属硫化物的组合物。
本发明是相对于我们已经公开的P.C.T.申请WO 99/33345的选择性发明。
所述WO99/33345公开了含有″THP″、与″THP″相容的非表面活性的生物渗透剂(biopenet rant)和任选的表面活性剂的增效杀生物组合物。
WO99/33345中将术语″THP″定义为四(羟烷基)盐或三(羟烷基)膦。为避免混淆，我们在下文中分别用″THP盐″或″THP″来指代。
所述WO 99/33345中公开的非表面活性的生物渗透剂的例子包括羧酸的膦酸化衍生物，如在我们已经公开的欧洲申请EP-A-0 491 391和EP-A-0 861 846中描述的膦酸化调聚物。
所述WO 99/33345中公开的其它非表面活性的生物渗透剂的例子包括N，N，N′，N′-四甲基-1，2-二氨基乙烷与二(2-氯乙基)醚的共聚物。该共聚物可以以商品名WSCP商购得到，下文中将以该商品名提及。
所述WO 99/33345中公开的视情况使用的表面活性剂的例子包括磺化(阴离子)表面活性剂和阳离子表面活性剂如基于季铵化合物的那些，以及非离子，两性和半极性表面活性剂。
我们现已出乎意料地发现当生物渗透剂是膦酸末端的聚合物或共聚物时，它与THP盐在一起产生增效作用，显著地提高了THP盐对浮游(自由游动)和固着的(附着的)细菌的杀生物效力。
还出乎意料地发现了当生物渗透剂是膦酸末端的聚合物或共聚物时，它与THP盐在一起产生增效作用，提高了THP盐对金属硫化物的溶解效力，尤其是硫化铁，锈。
因此，本发明提供了一种增效组合物，其包含：
(i)THP盐(如前述定义)和
(iii)生物渗透剂
其中生物渗透剂包含不饱和羧酸的聚合物或不饱和羧酸与磺酸的共聚物，所述聚合物或共聚物可以由单-或双-膦酸化不饱和羧酸封端或聚合物骨架的这类单体。
该增效组合物可以是增效杀生物组合物和/或增效溶解金属硫化物(如硫化铁)的组合物。
优选地，THP盐是硫酸四(羟甲基)磷盐(THPS)。其它THP盐包括亚磷酸盐，溴化物，氟化物，氯化物，磷酸盐，碳酸盐，乙酸盐，甲酸盐，柠檬酸盐，硼酸盐，和硅酸盐。
生物渗透剂可以包括不饱和羧酸的聚合物或不饱和羧酸和磺酸的共聚物，所述聚合物或共聚物可以由乙烯基膦酸(VPA)或乙烯叉基-1，1-二膦酸(VDPA)所封端或具有引入聚合物骨架的这类单体；相应地所述生物渗透剂可以是引入VPA和/或VDPA单体的无规共聚物。
生物渗透剂的聚合物或共聚物适宜地可以是聚丙烯酸酯或丙烯酸酯/磺酸酯共聚物。
根据本发明优选的实施方案，生物渗透剂可以是乙烯基膦酸封端的聚丙烯酸酯(以后称作″VPA封端的聚合物″)，或乙烯叉基-1，1-二膦酸封端的聚丙烯酸酯(以后称作″VDPA封端的聚合物″)，或引入VPA和/或VDPA单体的聚丙烯酸酯。
在其它优选的实施方案中，生物渗透剂可以是乙烯叉基-1，1-二膦酸封端的丙烯酸酯/磺酸酯共聚物(以后称作″VDPA封端的共聚物″)或乙烯基膦酸封端的丙烯酸酯/磺酸酯共聚物(以后称作″VPA封端的共聚物″)，或可以是引入VPA和/或VDPA单体的丙烯酸酯/磺酸酯共聚物。
在本发明的组合物中，当以重量百分比形式表示时，VPA或VDPA封端的聚合物或共聚物与THP盐的优选比例是0.5至50％，例如0.5至30％；优选1至25％，例如1至20％，例如1至10％或2至8％；最优选1至5％，例如3至5％(基于活性固体和含量为1-74％，例如50％的活性THP盐制剂)。
在一个实施方案中，生物渗透剂是VPA封端聚合物或VDPA封端共聚物。
当以重量百分比形式表示时，VPA封端的聚合物或VDPA封端的共聚物与THP盐的优选比例是0.5至50％，例如0.5至30％；优选1至25％，例如1至20％，例如1至10％或2至8％；最优选1至5％，例如3至5％(基于活性固体和含量为1-74％，例如50％的活性THP盐制剂)。
在一个实施方案中，该组合物可以以溶液形式提供，例如水溶液。
或者，该组合物可以以固体形式提供，例如通过将组分涂覆到或将组分吸附至粉状颗粒或多孔酸基质例如己二酸或通过掺入蜡状基质中形成的固体。
如上述所提及的，根据本发明组合物可以用作控制浮游(自由游动)和固着的(附着的)细菌的杀生物剂。
我们发现根据本发明组合物对于降低水中的常规异养菌和硫酸盐还原菌的水平同样有效。
因此，本发明还提供了一种处理已受或易受微生物如细菌，真菌或藻类污染的水系统的方法，其中该方法包括向所述系统分别或一起添加杀生物活性量的THP盐和生物渗透剂，其中生物渗透剂包括不饱和羧酸聚合物或不饱和羧酸和磺酸的共聚物，所述聚合物或共聚物由单-或二膦酸化不饱和羧酸基团封端或是含有单或二膦酸化不饱和羧酸的无规共聚物，从而至少杀死部分所述微生物。
水系统可以是例如被细菌粘液和/或浮游细菌所污染的。本发明可以用于处理需氧系统如冷却塔，纸加工系统和废水系统，还可以用于厌氧系统，如油井，如在二次开采过程中的油井。本发明还适合用于泥浆和官能流体的防腐，例如钻探泥浆、完井液、增产液和压裂液。
如上述所提及的，本发明的组合物还可以用于溶解金属硫化物，优选硫化铁；尤其是用于溶解硫化铁锈。然而，金属硫化物可以是硫化铅或硫化锌，或硫化铁或硫化铅与硫化锌的结合。
硫化铁典型地可以是硫铁矿(FeS)或黄铁矿(FeS2)，但任何一种硫化铁可以用本发明来加以溶解。
因此，本发明还提供了一种处理含有或与金属硫化物锈，如硫化铁锈相接触的水系统的方法，所述方法包括向所述系统分别或一起添加THP盐和生物渗透剂，其中所述生物渗透剂包括不饱和羧酸的聚合物或不饱和羧酸与磺酸的共聚物，所述聚合物或共聚物由单-或二-膦酸化的不饱和羧酸基团封端或是含有单-或二-膦酸化的不饱和羧酸的无规共聚物，从而至少溶解部分所述锈。
本发明可以用于石油和天然气工业，用于处理系统如油井，天然气井，管道，贮藏容器和生产设备，如在二次开采过程中，以及用于其它工业水系统，如在造纸工业系统中。
本发明将用以下实施例进行阐明。
在这些实施例中，各种缩写具有如下意义：
VPA聚合物：分子量约4000的乙烯基膦酸封端的聚丙烯酸酯
VDPA共聚物：分子量为5000-6000的乙烯叉基-二膦酸封端的丙烯酸酯/磺酸酯共聚物
GHB：常规异养菌
SRB：硫酸盐还原菌
WHO水：世界卫生组织标准硬水(参见下述表I)
SMOW水：标准普通海洋水(参见下述表II)
THPS：50％的硫酸四(羟甲基)
Figure 058039265_3
盐水溶液
WSCP：N，N，N′，N′-四甲基-1，2-二氨基乙烷和二(2-氯乙基)醚的共聚物
表IWHO标准硬水
1升含：CaCl2(无水)MgCl2.6H2O 0.305g0.139g
   表II标准普通海洋水
   5升含：NaClMgCl2.6H2ONa2SO4CaCl2.2H2OKClNaHCO3KBr 122.65g55.52g20.45g7.69g3.48g1.00g0.50g
   用0.1N NaOH将pH调至8.2
实施例1
在WHO水中的定量悬浮试验(浮游细菌)
试验产品     常规异养细菌的Log减少值(基于50ppm有效成分THPS)
    接触时间
    接触1小时     接触3小时
对照未配制的THPSTHPS/VPA聚合物*THPS/VDPA聚合物*THPS/0.7％WSCP     017.47.43.7     05.8全部杀死全部杀死7.4
实施例2
在脱墨废水中的定量悬浮试验
试验产品     75ppm有效成分THPS/接触3小时的Log减少值
    GHB     SRB
对照未配制的THPSTHPS/VPA聚合物*     03.85.1     033
实施例3
生物膜(固着的)试验：淡水(WHO)
  试验产品     75ppm有效成分THPS剂量接触3小时后的活细菌数(GHB)
  对照未配制的THPSTHPS/VPA聚合物*THPS/VDPA聚合物*THPS/2％磺化表面活性剂(a)     1×1051×1O51×105＜101×103
实施例4
生物膜试验：海水(SMOW)
  试验产品     75ppm有效成分THPS剂量接触3小时后的活细菌数
    GHB     SRB
  对照未配制的THPSTHPS/VPA聚合物*THPS/VDPA聚合物*THPS/5％季铵盐化合物(b)     1×1041×102＜101×1021×102     1×1061×104＜101×1021×103
*在每种情形下，THPS与″聚合物″的比例是50％有效成分THPS/5％″聚合物″，所述″聚合物″包含作为钠盐的25％固体。
(a)混合的单-和二-烷基二磺化二苯基氧化物的二-钠盐，以DOWFAX
Figure 058039265_4
2A1商购得到。
(b)烷基二甲基苄基氯化铵，以EMPIGENBAC 50商购得到。
实施例5
硫化铁溶解试验
制备下述溶液：
(a)THPS：-THPS(26.6g)+去离子水(73.4g)
(b)VPA聚合物：含20％活性成分的-VPA聚合物溶液(20g)+去离子水(80g)
(c)VDPA聚合物：含20％活性成分的-VDPA聚合物溶液(20g)+去离子水(80g)
(d)THPS/5％VPA聚合物：-THPS(26.6g)+含20％活性成分的VPA聚合物溶液(5g)+去离子水(68.4g)
(e)THPS/5％VDPA聚合物：-THPS(26.6g)+含20％活性成分的VDPA聚合物溶液(5g)+去离子水(68.4g)
(f)THPS/20％VPA聚合物：-THPS(26.6g)+含20％活性成分的VPA聚合物溶液(20g)+去离子水(53.4g)
(g)THPS/20％VDPA聚合物：-THPS(26.6g)+含20％活性成分的VDPA聚合物溶液(20g)+去离子水(53.4g)
向上述各溶液中加入2g(准确称量的)硫化铁场锈(field scale)(来自水注入系统)。接着将这些溶液在50℃的加热水浴中搅拌20小时，然后将它们通过一个称量过的滤纸来进行过滤。接着将滤纸和固体物在再次称量前干燥；由此测定剩余固体物的重量，计算损失的％重量。
还在Hach DR2000分光光度计上使用铁离子测定方法测定了滤液中铁离子浓度。
溶解剂 pH  ％重量损失  溶液中Fe2+浓度ppm
(a)THPS 3.23  63  3120
(b)VPA聚合物 4.54  60  1310
(c)VDPA聚合物 3.28  47  1430
(d)THPS+5％VPA聚合物 3.77  74  3320
(e)THPS+5％VDPA聚合物 3.13  78  3560
(f)THPS+20％VPA聚合物 3.94  76  3480
(g)THPS+20％VDPA聚合物 2.99  83  5260

Claims (16)

1.一种增效组合物，其包含：
(i)四(羟烷基)鏻盐和
(ii)生物渗透剂，
其中生物渗透剂是聚丙烯酸酯或丙烯酸酯和磺酸酯的共聚物，所述聚合物或共聚物由乙烯基膦酸VPA或乙烯叉基-1，1-二膦酸VDPA封端或者在所述聚合物或共聚物的聚合物骨架中引入有VPA或VDPA单体，
并且其中所述VPA或VDPA聚合物或共聚物的比例范围是1-50重量％，基于活性固体和1-74％四(羟烷基)鏻盐制剂。
2.如权利要求1的组合物，其中所述四(羟烷基)鏻盐是硫酸四(羟甲基)鏻盐。
3.如权利要求1的组合物，其中所述四(羟烷基)鏻盐是四(羟甲基)鏻的亚磷酸盐、溴化物、氟化物、氯化物、磷酸盐、碳酸盐、乙酸盐、甲酸盐、柠檬酸盐、硼酸盐或硅酸盐。
4.根据权利要求1的组合物，其中所述生物渗透剂是VPA封端的聚合物或VDPA封端的聚合物或引入VPA和/或VDPA单体的聚丙烯酸酯。
5.根据权利要求1的组合物，其中所述生物渗透剂是VDPA封端的共聚物或VPA封端的共聚物或引入VPA和/或VDPA单体的丙烯酸酯和磺酸酯的共聚物。
6.根据权利要求1的组合物，其中所述比例范围是1-25％重量。
7.根据权利要求6的组合物，其中所述比例范围是1-5％重量。
8.根据权利要求1-7任一所述的组合物用于制备杀生物剂的用途。
9.权利要求8的用途，其中所述杀生物剂用于控制浮游和/或固着的细菌。
10.权利要求8或9的用途，其中所述杀生物剂用于降低水中的常规异养菌和/或硫酸盐还原菌的水平。
11.一种处理已受或易受微生物污染的水系统的方法，其中该方法包括分别或一起向所述系统中加入杀生物有效量的四(羟烷基)鏻盐和生物渗透剂，其中生物渗透剂是聚丙烯酸酯或丙烯酸酯和磺酸酯的共聚物，所述聚合物或共聚物由乙烯基膦酸VPA或乙烯叉基-1，1-二膦酸VDPA封端或者在所述聚合物或共聚物的聚合物骨架中引入有VPA或VDPA单体，从而至少杀死部分所述微生物。
12.如权利要求11的方法，其中所述微生物选自细菌，真菌或藻类。
13.根据权利要求1-7任一所述的组合物用于溶解金属硫化物的用途。
14.权利要求13的用途，其中所述金属硫化物是硫化铁锈。
15.一种处理含有或接触金属硫化物锈的水系统的方法，其中该方法包括向所述系统中分别或同时加入四(羟烷基)鏻盐和生物渗透剂，其中生物渗透剂是聚丙烯酸酯或丙烯酸酯和磺酸酯的共聚物，所述聚合物或共聚物由乙烯基膦酸VPA或乙烯叉基-1，1-二膦酸VDPA封端或者在所述聚合物或共聚物的聚合物骨架中引入有VPA或VDPA单体，从而至少溶解部分所述锈。
16.权利要求15的方法，其中所述锈是硫化铁锈。
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