CN113181882A - 蛋白质基海水提铀复合吸附材料及其制备方法 - Google Patents
蛋白质基海水提铀复合吸附材料及其制备方法 Download PDFInfo
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Abstract
本发明公开了一种蛋白质基海水提铀复合吸附材料及其制备方法。在一定温度和pH条件下,将三(羟甲基)氨基甲烷和三(2‑羧乙基)膦共混调节pH值得到溶液①;将蛋白质与三(羟甲基)氨基甲烷共混,调节pH值,得到溶液②;将溶液①和溶液②比例混合,密封反应;反应开始进行时,立即加入基材,使基材充分浸泡在溶液中;得到基材用纯水洗涤数次,随后烘干即得干燥的蛋白质基复合吸附材料。本发明的制备方法简单、原材料丰富、反应条件温和,制备的材料吸附性能好,在海水提铀、放射性海水处理、回收贵金属、环境修复、工业废水处理等领域有着巨大的应用前景。
Description
技术领域
本发明涉及材料制备领域的一种复合吸附材料的制备方法,尤其涉及一种蛋白质基海水提铀复合吸附材料的制备方法。
背景技术
随着石油能源的逐渐枯竭,人们一直在寻找一种能够代替石油的新型能源,例如,热能、太阳能、风能等。热能得主要形式是将热能转化为热能,例如火力发电,虽然火力发电是当下应用范围最广的一种能源转换形式,但是在发电过程中会产生大量的温室气体,污染环境,因此并不能作为一种可持续发展的能源;太阳能、风能来源于大自然,发电过程中几乎不会污染环境,可持续性高,但是影响收集这两种能源的不可控因素过多,所产生的电量并不能满足当今社会所需要的电量,因此以现在的技术,太阳能、风能只能作为一种辅助能源。
核能源是目前全世界公认的,未来可以取代石油资源的新型能源,而且除了发生核泄漏这种意外以外,几乎不会产生污染。但是,核能源现在所面临的一个最大的问题就是:所需要的原料—铀,在陆地上的资源非常稀缺,经专家计算,陆地铀仅供人类使用一百年左右。因此,人类为了解决这个问题,将目光投向了海洋,对海洋中的铀含量进行了探测,结果发现,海洋中的铀含量大约有45亿吨,相当于可供人类使用一万年,但是海洋中的铀浓度过低,海水提铀成为了一大难题。
经过几十年的发展,人类发明了许多方法来提取海水中的铀,其中,吸附方法是公认最有效的方法。所谓吸附法就是利用吸附材料表面得功能基团去吸附海水中的铀酰离子,在众多的吸附材料中,复合吸附材料是现在研究的热门,因为复合材料不仅可以保持对铀很好的吸附能力,而且可以额外地优化其他性能,例如力学性能、亲水性能、抗菌性能等。
公开号为CN108579709A的中国专利公开了一种用于海水提铀的多孔结构弹性复合材料制备方法,将偕胺肟化聚丙烯腈溶液与强碱混溶;将混合溶液加入到能够交联凝胶化的高分子材料溶液中;将多孔结构弹性材料浸没到混合溶液中,真空脱气泡;干燥;将干燥后的多孔结构弹性材料浸没于交联剂溶液中进行交联凝胶化;用清水漂洗,即得。本发明通过能够交联凝胶化的高分子材料水溶液进行交联凝胶化复合,提高了偕胺肟化聚丙烯腈在多孔结构弹性材料骨架上的包覆强度、改善材料柔性、力学稳定性和亲水性。
公开号为CN110256550A的中国专利公开了一种用于海水提铀的重组蛛丝蛋白纤维材料的制备方法,包括以下步骤:将蜘蛛丝蛋白基因片段、海水提铀功能蛋白基因片段和柔性连接基因重组获得海水提铀重组蛛丝蛋白编码基因;后转入大肠杆菌,经蛋白表达、纯化获得海水提铀重组蛛丝蛋白液;浓缩使其浓度为100-300mg/mL,将浓缩后的海水提铀重组蛛丝蛋白液推进纺丝液,自组装获得海水提铀重组蛛丝蛋白纤维;所述纺丝液的pH为3-5。本方法工艺简单,条件温和,易于纯化,且通过本方法制备的海水提铀重组蛛丝蛋白纤维材料,力学性能优异,铀吸附能力强且选择性高,可多次重复使用。
公开号为CN109999761A的中国专利公开了一种聚乙烯亚胺树脂复合材料的制备方法及应用,所述复合材料为PEI接枝到含氯树脂上的PEI改性树脂,通过将PEI接枝到含氯树脂上制备得到,用作铀的吸附材料。所述材料中PEI 有良好的水稳定性和亲水性,且具有大量氨基和亚氨基,这些基团均具有配位能力,可以用于吸附,对铀酰离子具有较大的吸附量,在海水提铀领域有着广阔的应用前景。
公开号为CN108745320A的中国专利公开了一种基于海水提铀的纳米明胶/ 聚合物复合纤维带的制备方法,包括:步骤一、纳米明胶/聚合物纤维带的制备,即将明胶和聚合物分别溶解,按比例混合,搅拌均匀后制成纺丝溶液,静电纺丝、干燥、裁剪,得纳米明胶/聚合物纤维带;步骤二、单宁固化,将明胶/聚合物纤维带浸泡于单宁水溶液中1-10h后,取出,再将其转入蒸馏水中,搅拌,加入交联剂,于温度20~50℃交联2-6h,再取出、洗涤、干燥,制得固化单宁的纳米明胶/聚合物复合纤维带。该纤维带由纳米级纤维编制而成,纤维直径小,比表面积大,固化单宁量多,对低浓度铀具有极高的选择性吸附能力;且其水力学性能、漂浮性、与水涌动性能好,可广泛用于海水、盐湖及放射性废水中铀的分离富集。
已经报道的复合吸附材料的制备方法中,最关键的步骤是材料的复合,方法①:通过交联凝胶化将两种材料交联在一起;方法②:两种材料的蛋白基因切片并重组成新的蛋白基因;方法③:将一种材料接枝到另一种材料的表面;方法④:两种材料静电混纺成纤维后交联。总的来说,这几种方法制备步骤多,反应复杂,而且某些原材料价格昂贵,使得无法投入到实际的应用当中。
发明内容
由于蛋白质由多种氨基酸组成,因此其表面含有多种功能基团,例如胺基、羧基、羟基等,使得其对铀着优异的吸附性能以及亲水性,进一步与比表表面积大的多孔材料复合,可以提高其力学性能,功能基团的分布面积等。有鉴于此,本发明提供了一种步骤简单、经济可行、原料丰富、应用范围广的蛋白质基复合吸附材料。
本发明基于通过TCEP将蛋白质中的二硫键的破坏,使得蛋白质小分子重新聚集,进而使这些小分子负载在溶液中的基材表面上;取出基材洗涤并烘干;所得材料即为蛋白质基复合吸附材料。通过控制蛋白质的种类、基材种类、TCEP 与蛋白质的质量比、基材浸泡时间来调节蛋白质基吸附材料的吸附性能。
本发明所采用的技术方案是:
(1)在10℃~60℃和pH=6~10的条件下,将三(羟甲基)氨基甲烷 (Tris-HCl)和三(2-羧乙基)膦(TCEP)共混0.1~2小时,调节pH值为6~9,得到溶液①;
在10℃~60℃和pH=5~9的条件下,将蛋白质与三(羟甲基)氨基甲烷共混 0.1~2小时,调节pH值为6~9,得到溶液②;
(2)在10~60℃,pH=5~10的条件下,将溶液①和溶液②按一定比例混合,密封反应0.1~12小时;
(3)上述反应开始进行时,立即加入基材,使基材充分浸泡在溶液中,在 30℃下反应0.1~12小时,反应过程中,不断滴加HCl溶液使pH维持在6.4~ 7.4;
(4)将(3)得到的基材用纯水洗涤数次,随后烘干6小时,即得干燥的蛋白质基复合吸附材料。
所述步骤(1)所涉及的蛋白质为溶菌酶、卵清蛋白、牛血清蛋白、免疫球蛋白、乳铁蛋白、金属硫蛋白、大豆蛋白、超氧化物歧化酶(SOD)、丝胶蛋白、丝素蛋白中的至少一种。
所述步骤(1)中,三(2-羧乙基)膦(TCEP)质量范围在0.12~204g,三(羟甲基)氨基甲烷(Tris-HCl)质量范围在0.01~17g。
所述步骤(2)中,蛋白质的质量范围在0.04~68g,蛋白质和三(羟甲基) 氨基甲烷的质量配比关系是3~6:1。
所述步骤(2)中,溶液①与溶液②的体积比为1:1~20。
所述步骤(1)所涉及的蛋白质为溶菌酶、卵清蛋白、牛血清蛋白、免疫球蛋白、乳铁蛋白、金属硫蛋白、大豆蛋白、超氧化物歧化酶(SOD)、丝胶蛋白、丝素蛋白中的至少一种。
所述步骤(3)中所述的基材为纳米海绵、氧化石墨烯、碳纳米管、Fe3O4、巴沙木、椴木、COFs、MOFs、PoPs中的至少一种。
所述步骤(3)中基材的浸泡的时间范围为0.1~24小时。
所制备的蛋白质基复合吸附材料表面负载其他的聚合物、功能基团等,使得其可以进一步优化固有的性能或者增加更多优异的性能。
所制备的蛋白质基复合吸附材料用于海水提铀、放射性海水处理、贵金属回收、环境修复、工业废水处理等。
本发明具有如下优点和有益效果:
所需要的原材料、基材种类丰富,来源范围广,成本低且对铀有着优异的吸附性能。同时,整个操作过程简单,反应条件(如,温度、PH、反应时间等) 温和。此外,所制备的复合材料可以引入更多的功能基团或者负载其他的聚合物以优化其性能,同时也为复合吸附材料的制备领域添加了新的制备方法。
用本方法制备的复合材料在海水提铀、放射性海水处理、回收贵金属、环境修复、工业废水处理等领域有着巨大的应用前景。
附图说明
图1是不同原料对铀的吸附性能图;
图2是不同基材对铀的吸附性能图;
图3是TCEP与原料的质量比对铀的吸附性能图;
图4是不同pH对铀的吸附性能图。
具体实施方式
通过以下实施例对本发明做更详细的描述,但所述实施例不构成对本发明的限制。
本发明的实施例如下:
实施例1
选用溶菌酶为反应所需要的蛋白质原料,纳米海绵作为基材。在温度为30℃的条件下,将0.0242g Tris-HCl与0.2866g TCEP加入到20ml纯水中充分混合,混合后调节pH值为8.4,得到溶液①;在温度为30℃的条件下,将0.0242g Tris-HCl与0.08g溶菌酶加入到20ml纯水中充分混合,混合后调节pH值为7.4,得到溶液②;将溶液①与溶液②混合后,立即将纳米海绵放入混合液中,在30℃下反应2小时,反应过程中,通过自动滴定系统不断滴加0.1mol/L HCl溶液使pH维持在7;反应结束后,将纳米海绵取出,洗涤数次后烘干得到蛋白质基复合吸附材料。
将干燥后的纳米海绵加入到浓度为16ppm,pH值为6的铀酰离子水溶液中,置于振荡器中震荡12小时后用ICP-MS测试溶液中铀酰离子的含量。经测试分析,蛋白质基纳米海绵对铀酰离子的吸附量为:1007.3mg/g。
实施例2~10
分别选用卵清蛋白、牛血清蛋白、免疫球蛋白、乳铁蛋白、金属硫蛋白、大豆蛋白、超氧化物歧化酶(SOD)、丝胶蛋白、丝素蛋白作为蛋白质原料,其余条件同实例1。结果显示,牛血清蛋白基纳米海绵有一个更好的吸附性能(见图2)。
实施例11~18
分别选用氧化石墨烯、碳纳米管、Fe3O4、巴沙木、椴木、COFs、MOFs、 PoPs作为基材,其余条件同实例1。结果显示,蛋白质基Fe3O4的吸附性能最好 (见图3)。
实施例19~24
TCEP与溶菌酶的质量比分别为1:1、2:1、3:1、4:1、5:1、6:1,其余条件同实施例1。结果显示,TCEP与溶菌酶的质量比为3:1时,吸附性能最佳(见图 3)。
实施例25~30
分别将浓度为16ppm的铀酰离子水溶液的pH值调节为1~11,其余条件同实施例1。结果显示,该吸附材料在pH范围在4~8对铀的吸附含量高达1000 以上。
由此实施可见,本发明制备的材料吸附性能好,制备方法简单、原材料丰富、反应条件温和,在海水提铀、放射性海水处理、回收贵金属、环境修复、工业废水处理等领域进行充分应用。
Claims (10)
1.一种蛋白质基海水提铀复合吸附材料的制备方法,其特征在于:包括以下步骤:
(1)在10℃~60℃和pH=6~10的条件下,将三(羟甲基)氨基甲烷和三(2-羧乙基)膦共混0.1~2小时,调节pH值为6~9,得到溶液①;
在10℃~60℃和pH=5~9的条件下,将蛋白质与三(羟甲基)氨基甲烷共混0.1~2小时,调节pH值为6~9,得到溶液②;
(2)在10~60℃,pH=5~10的条件下,将溶液①和溶液②按一定比例混合,密封反应0.1~12小时;
(3)上述反应开始进行时,立即加入基材,使基材充分浸泡在溶液中,在30℃下反应0.1~12小时,反应过程中,不断滴加HCl溶液使pH维持在6.4~7.4;
(4)将(3)得到的基材用纯水洗涤数次,随后烘干6小时,即得干燥的蛋白质基复合吸附材料。
2.根据权利要求1所述的蛋白质基海水提铀复合吸附材料的制备方法,其特征在于:所述步骤(1)所涉及的蛋白质为溶菌酶、卵清蛋白、牛血清蛋白、免疫球蛋白、乳铁蛋白、金属硫蛋白、大豆蛋白、超氧化物歧化酶、丝胶蛋白、丝素蛋白中的至少一种。
3.根据权利要求1所述的蛋白质基海水提铀复合吸附材料的制备方法,其特征在于:所述步骤(1)中,三(2-羧乙基)膦质量范围在0.12~204g,三(羟甲基)氨基甲烷质量范围在0.01~17g。
4.根据权利要求1所述的蛋白质基海水提铀复合吸附材料的制备方法,其特征在于:所述步骤(2)中,蛋白质的质量范围在0.04~68g,蛋白质和三(羟甲基)氨基甲烷的质量配比关系是3~6:1。
5.根据权利要求1所述的蛋白质基海水提铀复合吸附材料的制备方法,其特征在于:所述步骤(2)中,溶液①与溶液②的体积比为1:1~20。
6.根据权利要求1所述的蛋白质基海水提铀复合吸附材料的制备方法,其特征在于:所述步骤(1)所涉及的蛋白质为溶菌酶、卵清蛋白、牛血清蛋白、免疫球蛋白、乳铁蛋白、金属硫蛋白、大豆蛋白、超氧化物歧化酶、丝胶蛋白、丝素蛋白中的至少一种。
7.根据权利要求1所述的蛋白质基海水提铀复合吸附材料的制备方法,其特征在于:所述步骤(3)中所述的基材为纳米海绵、氧化石墨烯、碳纳米管、Fe3O4、巴沙木、椴木、COFs、MOFs、PoPs中的至少一种。
8.根据权利要求1所述的蛋白质基海水提铀复合吸附材料的制备方法,其特征在于:所述步骤(3)中基材的浸泡的时间范围为0.1~24小时。
9.一种蛋白质基海水提铀复合吸附材料,其特征在于:
所述的复合吸附材料采用权利要求书1-8任一所述制备方法制备而成。
10.根据权利要求9所述的一种蛋白质基海水提铀复合吸附材料的应用,其特征在于:所制备的蛋白质基复合吸附材料用于海水提铀、放射性海水处理、贵金属回收、环境修复、工业废水处理等。
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