CN109622041A - 一种双组分、多重网络纳米纤维气凝胶负载异质结光催化剂的制备方法及应用 - Google Patents
一种双组分、多重网络纳米纤维气凝胶负载异质结光催化剂的制备方法及应用 Download PDFInfo
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- CN109622041A CN109622041A CN201910072377.0A CN201910072377A CN109622041A CN 109622041 A CN109622041 A CN 109622041A CN 201910072377 A CN201910072377 A CN 201910072377A CN 109622041 A CN109622041 A CN 109622041A
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Abstract
本发明属于纳米功能材料制备及其应用领域,特别涉及一种双组分、多重网络纳米纤维气凝胶负载异质结光催化剂的制备方法及应用;本发明一方面利用高压静电纺丝技术和氨基功能化处理制得氨化高分子纳米纤维;另一方面从天然植物中提取纤维素纳米纤维,利用两种纳米纤维之间的氢键作用交叉形成三维网络气凝胶,制得双组分、多重网络纳米纤维气凝胶;利用水热法,在其三维网络结构中生长异质结光催化剂;本发明制备的气凝胶光催化剂,热稳定性强,形貌可控,制备流程简单,便于大规模生产;其轻质,亲水的特点,结合其多重网络结构中生长的异质结催化剂,对水环境中典型污染物都具有很好的转化去除效果,与此同时,还具备产氢和杀菌功能。
Description
技术领域
本发明属于纳米功能材料制备及其应用领域,特别涉及一种双组分、多重网络纳米纤维气凝胶负载异质结光催化剂的制备方法及应用。
背景技术
随着社会工业的不断发展,水体环境污染问题日益突出。人们对水体环境污染物的去除从一般意义上的吸附、沉淀、萃取等污染物分离转移方式向无害化方向转变。其中,光催化作为一种高级氧化技术,因具有能耗低,无二次污染,效率高等优点,逐渐成为目前的研究热点。光催化剂,作为光催化技术过程的核心,对光催化效率影响巨大。目前,常用的光催化剂以纳米颗粒和粉末为主,易团聚,难分离,容易造成二次污染,且单一组分的光催化剂具有光吸收范围窄,效率低,电子、空穴复合速度快等缺点。
因此,需要开发新型催化剂载体,并通过金属/非金属掺杂、构建异质结等方式解决现有光催化剂的不足。常用的催化剂载体包括玻璃、陶瓷、膜、微球等,这些载体均存在一定程度的不足,例如,玻璃载体厚重,表面光滑,实际使用不便;而陶瓷载体较为昂贵;膜载体形貌和孔径调控难度大,运行成本高;微球载体需要外加磁性或过滤等方式回收,操作不便。纳米纤维气凝胶,作为一种轻质、低密度材料,其独特的网络结构和孔隙,使其成为光催化剂的良好载体。然而,一般的天然纤维素气凝胶存在热稳定性差、机械强度不高等问题,限制其在负载光催化剂方面的应用范围。
发明内容
本发明旨在解决现有技术中存在的上述技术问题,提供了一种双组分、多重网络纳米纤维气凝胶负载异质结光催化剂的制备方法,将高分子聚合物纳米纤维进行胺化后,与天然纤维素纳米纤维通过氢键作用构筑具有多重网络结构的气凝胶、水热生长石墨氮化碳与铁系金属有机框架材料形成异质结,复合制备出高效去除水体多种污染物的气凝胶光催化剂。
为解决上述问题,本发明的技术方案如下:
一种双组分、多重网络纳米纤维气凝胶负载异质结光催化剂的制备方法,包括以下步骤:
步骤1,制备氨化的聚丙烯腈纳米纤维;
步骤2,将所述氨化的聚丙烯腈纳米纤维分散在水溶液中,制得溶液A;将纤维素纳米纤维分散在水溶液中,制得溶液B;将溶液A与溶液B混合、加热、冻干,制得双组分、多重网络纳米纤维气凝胶;
步骤3,取石墨氮化碳,铁源试剂,二氨基对苯二甲酸,步骤2制得的双组分、多重网络纳米纤维气凝胶,加入N,N-二甲基甲酰胺溶剂中,水热反应8~24小时,制得产物。
优选地,步骤1所述氨化的高分子聚合物纳米纤维的制备方法为:
步骤1.1,以聚丙烯腈高分子聚合物溶液为纺丝液,利用高压静电纺丝技术制备聚丙烯腈纳米纤维;
步骤1.2,将所述聚丙烯腈纳米纤维置于含氨化试剂的水溶液中,调节温度为100~180℃,加热反应6~24小时。
优选地,所述步骤1.1中,纺丝液的质量分数为8%~15%,纺丝电压为10~30kV,纺丝液体流速为0.5~2.0mL/h,收集距离为13~22cm。
优选地,所述步骤1.2中,聚丙烯腈纳米纤维的投加量为2g/L~5g/L,氨化试剂的投加量为100g/L~500g/L。
优选地,所述步骤1.2中,氨化试剂为乙二胺、三乙烯二胺、四乙烯五胺,多胺、聚乙烯亚胺中的任意一种。
优选地,所述步骤2中,加热条件为:置于烘箱中80℃烘0.5~8小时。
优选地,所述步骤2中,溶液A中氨化的聚丙烯腈纳米纤维与水的质量体积比为5g/L~20g/L,溶液B中质量分数为5%的纤维素纳米纤维溶液与水的体积比为1:5~1:20,溶液A与溶液B的混合体积比为1:1。
优选地,步骤3中,所述石墨氮化碳的制备方法为:将三聚氰胺在400~550℃条件下,煅烧2~6小时。
优选地,所述步骤3中,铁源试剂为硝酸铁、氯化铁、硫酸铁中的任意一种。
优选地,所述步骤3中,石墨氮化碳的投加量为1~5g/L,铁源试剂的投加量为2~10g/L,铁源试剂与二氨基对苯二甲酸的质量比为1:1~1:5,纳米纤维气凝胶的投加量为0.5~2g/L。
优选地,所述步骤3中,水热反应温度为120~180℃。
优选地,所述步骤3中,所得产物的后处理方法为:用乙醇和水清洗干净,于真空干燥箱60℃烘干。
本发明利用天然纤维素纳米纤维的羟基和高分子聚合物纳米纤维的氨基之间的氢键作用以及两组分之间交叉形成的多重网络结构,提高气凝胶载体的热稳定性和机械性能,且结构形貌可控;将石墨氮化碳与铁系金属有机框架材料进行复合,构建异质结,从而提高电子与空穴的分离效率,增强光催化效果;同时,通过水热生长的方式,将石墨氮化碳与铁系金属有机框架材料负载到双组分、多重网络纳米纤维气凝胶;该双组分、多重网络纳米纤维气凝胶负载异质结光催化剂可用于高效去除水体多种污染物;同时还可以用于产氢和水体杀菌。
相对于现有技术,本发明的优点如下,
1)与现有的光催化剂相比,本发明所制备的三维气凝胶催化剂,可见光区域吸收性能明显增强,电子空穴分离效率高。
2)相比较大多数粉体催化剂,新制备的三维气凝胶催化剂,解决了目前纳米颗粒和粉体光催化剂易团聚,难回收的问题,可循环重复使用多次,无二次污染。
3)采用双组分、多重网络纳米纤维气凝胶为载体,构筑多重网络结构,解决现有气凝胶载体的热稳定性差,机械强度不高等问题,从而拓宽其应用范围。
附图说明
图1是本发明实施例3涉及的复合光催化剂的实物图;
图2是本发明实施例3涉及的复合光催化剂的扫描电镜图;
图3是本发明实施例3所制备的双组分、多重网络气凝胶载体与纤维素纳米纤维载体的热稳定性对比图;
图4是本发明实施例3所制备的双组分、多重网络气凝胶修饰催化剂前后的应力-应变曲线图;
图5是本发明实施例1-6所制备的复合光催化剂对六价铬的还原效果图;
图6是本发明实施例3所制备的复合光催化剂对磺胺甲恶唑的降解效果图;
图7是本发明实施例3所制备的复合光催化剂对六价铬还原的循环使用效果图;
图8是本发明实施例3所制备的复合光催化剂对磺胺甲恶唑降解的重复使用效果图;
图9是本发明实施例3所制备的复合光催化剂、石墨氮化碳、铁系金属有机框架材料的产氢效果对比图;
图10是本发明实施例3所制备的复合光催化剂的杀菌效果图。
具体实施方式
实施例1
一种双组分、多重网络纳米纤维气凝胶负载异质结光催化剂的制备方法,其制备步骤如下:
1)配制8%聚丙烯腈高分子聚合物溶液,固定在高压静电纺丝机的注射泵上,纺丝机的负极与收集板相连,正极与玻璃注射器相连,调节电压为10kv,正负极距离为13cm,流速为0.5mL/h,利用高压静电纺丝技术制备出纳米纤维;
2)称取0.4g步骤1)所制备的纳米纤维置于含聚乙烯亚胺的200ml水溶液中,其中聚乙烯亚胺的投加量为20g,调节温度为100℃,加热反应6小时;
3)将步骤2)中氨化后的纳米纤维取出,用乙醇和水冲洗去除残留的聚乙烯亚胺,置于真空干燥箱中60℃烘24小时;
4)称取0.05g步骤3)得到的氨化纳米纤维,加入10mL水溶液中,高速搅拌分散混匀,设为溶液A;取纤维素纳米纤维水溶液(纤维素纳米纤维的质量分数为5%)2mL,稀释分散于10mL水溶液中,设为溶液B;将溶液A和溶液B混合均匀后,置于烘箱中80℃烘0.5小时,转移至冷冻干燥机中抽干,即得双组分、多重网络纳米纤维气凝胶;
5)称取2g的三聚氰胺,置于马弗炉中,于400℃煅烧2小时,得石墨氮化碳粉末;
6)称取石墨氮化碳0.05g,硝酸铁0.1g,二氨基对苯二甲酸0.1g,双组分、多重网络纳米纤维气凝胶25mg,加入50mL N,N-二甲基甲酰胺溶剂中,置于反应釜中,120℃水热反应8小时;将得到的复合光催化剂用乙醇和水清洗干净,于真空干燥箱中60℃烘干。
实施例2
一种双组分、多重网络纳米纤维气凝胶负载异质结光催化剂的制备方法,其制备步骤如下:
1)配制15%聚丙烯腈高分子聚合物溶液,固定在高压静电纺丝机的注射泵上,纺丝机的负极与收集板相连,正极与玻璃注射器相连,调节电压为30kv,正负极距离为22cm,流速为2.0mL/h,利用高压静电纺丝技术制备出纳米纤维;
2)称取1.0g步骤1)所制备的纳米纤维置于含三乙烯二胺的200ml水溶液中,其中三乙烯二胺的投加量为100g,调节温度为180℃,加热反应24小时;
3)将步骤2)中氨化后的纳米纤维取出,用乙醇和水冲洗去除残留的三乙烯二胺,置于真空干燥箱中60℃烘24小时;
4)称取0.2g步骤3)得到的氨化纳米纤维,加入10mL水溶液中,高速搅拌分散混匀,设为溶液A;取纤维素纳米纤维水溶液(纤维素纳米纤维的质量分数为5%)0.5mL,稀释分散于10mL水溶液中,设为溶液B;将溶液A和溶液B混合均匀后,置于烘箱中80℃烘8小时,转移至冷冻干燥机中抽干,即得双组分、多重网络纳米纤维气凝胶;
5)称取2g的三聚氰胺,置于马弗炉中,于550℃煅烧6小时,得石墨氮化碳粉末;
6)称取石墨氮化碳0.25g,硫酸铁0.5g,二氨基对苯二甲酸2.5g,双组分、多重网络纳米纤维气凝胶100mg,加入50mL N,N-二甲基甲酰胺溶剂中,置于反应釜中,180℃水热反应24小时;将得到的复合光催化剂用乙醇和水清洗干净,于真空干燥箱60℃烘干。
实施例3
一种双组分、多重网络纳米纤维气凝胶负载异质结光催化剂的制备方法,其制备步骤如下:
1)配制10%聚丙烯腈高分子聚合物溶液,固定在高压静电纺丝机的注射泵上,纺丝机的负极与收集板相连,正极与玻璃注射器相连,调节电压为20kv,正负极距离为15cm,流速为1.0mL/h,利用高压静电纺丝技术制备出纳米纤维;
2)称取0.6g步骤1)所制备的纳米纤维置于含四乙烯五胺的200ml水溶液中,其中四乙烯五胺的投加量为40g,调节温度为150℃,加热反应12小时;
3)将步骤2)中氨化后的纳米纤维取出,用乙醇和水冲洗去除残留的四乙烯五胺,置于真空干燥箱中60℃烘24小时;
4)称取0.1g步骤3)得到的氨化纳米纤维,加入10mL水溶液中,高速搅拌分散混匀,设为溶液A;取纤维素纳米纤维水溶液(纤维素纳米纤维的质量分数为5%)1mL,稀释分散于10mL水溶液中,设为溶液B;将溶液A和溶液B混合均匀后,置于烘箱中80℃烘4小时,转移至冷冻干燥机中抽干,即得双组分、多重网络纳米纤维气凝胶;
5)称取2g的三聚氰胺,置于马弗炉中,于500℃煅烧4小时,得石墨氮化碳粉末;
6)称取石墨氮化碳0.1g,氯化铁0.3g,二氨基对苯二甲酸0.6g,双组分、多重网络纳米纤维气凝胶50mg,加入50mL N,N-二甲基甲酰胺溶剂中,置于反应釜中,150℃水热反应12小时;将得到的复合光催化剂用乙醇和水清洗干净,于真空干燥箱60℃烘干。
实施例4
一种双组分、多重网络纳米纤维气凝胶负载异质结光催化剂的制备方法,其制备步骤如下:
1)配制15%聚丙烯腈高分子聚合物溶液,固定在高压静电纺丝机的注射泵上,纺丝机的负极与收集板相连,正极与玻璃注射器相连,调节电压为30kv,正负极距离为22cm,流速为2.0mL/h,利用高压静电纺丝技术制备出纳米纤维;
2)称取1.0g步骤1)所制备的纳米纤维置于含聚乙烯亚胺的200ml水溶液中,其中聚乙烯亚胺的投加量为100g,调节温度为180℃,加热反应24小时;
3)将步骤2)中氨化后的纳米纤维取出,用乙醇和水冲洗去除残留的聚乙烯亚胺,置于真空干燥箱中60℃烘24小时;
4)称取0.2g步骤3)得到的氨化纳米纤维,加入10mL水溶液中,高速搅拌分散混匀,设为溶液A;取纤维素纳米纤维水溶液(纤维素纳米纤维的质量分数为5%)0.5mL,稀释分散于10mL水溶液中,设为溶液B;将溶液A和溶液B混合均匀后,置于烘箱中80℃烘8小时,转移至冷冻干燥机中抽干,即得双组分、多重网络纳米纤维气凝胶;
5)称取2g的三聚氰胺,置于马弗炉中,于550℃煅烧6小时,得石墨氮化碳粉末;
6)称取石墨氮化碳0.25g,氯化铁0.5g,二氨基对苯二甲酸2.5g,双组分、多重网络纳米纤维气凝胶100mg,加入50mL N,N-二甲基甲酰胺溶剂中,置于反应釜中,180℃水热反应24小时;将得到的复合光催化剂用乙醇和水清洗干净,于真空干燥箱中60℃烘干。
实施例5
一种双组分、多重网络纳米纤维气凝胶负载异质结光催化剂的制备方法,其制备步骤如下:
1)配制10%聚丙烯腈高分子聚合物溶液,固定在高压静电纺丝机的注射泵上,纺丝机的负极与收集板相连,正极与玻璃注射器相连,调节电压为20kv,正负极距离为15cm,流速为1.0mL/h,利用高压静电纺丝技术制备出纳米纤维;
2)称取0.6g步骤1)所制备的纳米纤维置于含乙二胺的200ml水溶液中,其中乙二胺的投加量为40g,调节温度为150℃,加热反应12小时;
3)将步骤2)中氨化后的纳米纤维取出,用乙醇和水冲洗去除残留的乙二胺,置于真空干燥箱中60℃烘24小时;
4)称取0.1g步骤3)得到的氨化纳米纤维,加入10mL水溶液中,高速搅拌分散混匀,设为溶液A;取纤维素纳米纤维水溶液(纤维素纳米纤维的质量分数为5%)1mL,稀释分散于10mL水溶液中,设为溶液B;将溶液A和溶液B混合均匀后,置于烘箱中80℃烘4小时,转移至冷冻干燥机中抽干,即得双组分、多重网络纳米纤维气凝胶;
5)称取2g的三聚氰胺,置于马弗炉中,于500℃煅烧4小时,得石墨氮化碳粉末;
6)称取石墨氮化碳0.1g,氯化铁0.3g,二氨基对苯二甲酸0.6g,双组分、多重网络纳米纤维气凝胶50mg,加入50mL N,N-二甲基甲酰胺溶剂中,置于反应釜中,150℃水热反应12小时;将得到的复合光催化剂用乙醇和水清洗干净,于真空干燥箱60℃烘干。
实施例6
一种双组分、多重网络纳米纤维气凝胶负载异质结光催化剂的制备方法,其制备步骤如下:
1)配制8%聚丙烯腈高分子聚合物溶液,固定在高压静电纺丝机的注射泵上,纺丝机的负极与收集板相连,正极与玻璃注射器相连,调节电压为10kv,正负极距离为13cm,流速为0.5mL/h,利用高压静电纺丝技术制备出纳米纤维;
2)称取0.4g步骤1)所制备的纳米纤维置于含四乙烯五胺的200ml水溶液中,其中四乙烯五胺的投加量为20g,调节温度为100℃,加热反应6小时;
3)将步骤2)中氨化后的纳米纤维取出,用乙醇和水冲洗去除残留的四乙烯五胺,置于真空干燥箱中60℃烘24小时;
4)称取0.05g步骤3)得到的氨化纳米纤维,加入10mL水溶液中,高速搅拌分散混匀,设为溶液A;取纤维素纳米纤维水溶液(纤维素纳米纤维的质量分数为5%)2mL,稀释分散于10mL水溶液中,设为溶液B;将溶液A和溶液B混合均匀后,置于烘箱中80℃烘0.5小时,转移至冷冻干燥机中抽干,即得双组分、多重网络纳米纤维气凝胶;
5)称取2g的三聚氰胺,置于马弗炉中,于400℃煅烧2小时,得石墨氮化碳粉末;
6)称取石墨相石墨氮化碳0.05g,硝酸铁0.1g,二氨基对苯二甲酸0.1g,双组分、多重网络纳米纤维气凝胶25mg,加入50mL N,N-二甲基甲酰胺溶剂中,置于反应釜中,120℃水热反应8小时;将得到的复合光催化剂用乙醇和水清洗干净,于真空干燥箱中60℃烘干。
验证实验1
将25mg实施例1-6制备的光催化剂置于50mL、浓度为10mg/L的六价铬溶液中,黑暗条件下预吸附半小时,开启500W氙灯进行光照,间隔一定时间取样,用紫外分光光度计于波长540nm处测定吸光度。还原曲线如图5所示,从图上可以看出,本发明所制备的复合光催化剂对六价铬具有快速高效还原的特点。其中,实施例3对六价铬的还原效果最佳。因此,选择实施例3的制备方法所制备的复合光催化剂进行验证实验2-6.
验证实验2
将25mg实施例3制备的光催化剂置于50mL、浓度为20mg/L的磺胺甲恶唑溶液中,黑暗条件下预吸附半小时,开启500W氙灯进行光照,间隔一定时间取样,用液相色谱测定计算其浓度。氧化曲线如图6所示,从图上可以看出,本发明所制备的复合光催化剂对磺胺甲恶唑具有快速高效降解的特点。
验证实验3
将25mg实施例3制备的光催化剂置于50mL、浓度为10mg/L的六价铬溶液中,黑暗条件下预吸附半小时,开启500W氙灯进行光照一小时后,取样于波长540nm处测定吸光度并计算六价铬的剩余浓度,将第一次使用后的复合光催化剂去除,烘干,进行循环重复使用实验,实验条件同第一次,结果如图7所示,从图上可以看出,本发明所制备的复合光催化剂对六价铬的还原能够重复多次进行,还原效果没有明显降低。
验证实验4
将25mg实施例3制备的光催化剂置于50mL、浓度为20mg/L的磺胺甲恶唑溶液中,黑暗条件下预吸附半小时,开启500W氙灯进行光照两小时后,取样用液相色谱测定并计算其的剩余浓度,将第一次使用后的复合光催化剂取出,烘干,进行循环重复使用实验,实验条件同第一次,结果如图8所示,从图上可以看出,本发明所制备的复合光催化剂对磺胺甲恶唑的降解能够重复多次进行,降解效果没有明显降低。
验证实验5
分别称取0.1g实施例3制备的复合光催化剂,单组份铁系金属有机框架材料和石墨氮化碳置于240mL的水溶液中,加入30mL三乙醇胺,超声混匀后,加入3wt%Pt,开启500W氙灯进行光照,每隔1小时,用气相色谱在线监测所产生的氢气浓度,结果如图9所示,本发明所制备的复合光催化剂的产氢量均高于单组份光催化剂。
验证实验6
称取三份50mL、等浓度的鼠伤寒沙门氏菌TA1535菌液,一份加入25mg实施例3制备的复合光催化剂,用500W氙灯进行光照2小时,编号为I;一份不加光催化剂,用500W氙灯进行光照2小时,编号为II;一份不加光催化剂,于黑暗条件下放置2小时,编号为III。鼠伤寒沙门氏菌TA98的操作过程同TA1535,其结果如图10所示,从图上可以看出,本发明所制备的复合光催化剂对鼠伤寒沙门氏菌的杀菌效果明显。
结合实施例1~6和验证实验1~6,采用本发明提供的制备方法制备得到的复合光催化剂,可以快速高效用于水体多种环境污染物的去除,稳定性强,可多次重复使用,除此之外,还具有产氢和杀菌效果。本发明提供的制备方法简便易行,能耗低,在水体中污染物降解方面具有广阔的应用前景。
需要说明的是上述实施例仅仅是本发明的较佳实施例,并没有用来限定本发明的保护范围,在上述基础上做出的等同替换或者替代均属于本发明的保护范围。
Claims (10)
1.一种双组分、多重网络纳米纤维气凝胶负载异质结光催化剂的制备方法,其特征在于,包括以下步骤:
步骤1,制备氨化的聚丙烯腈纳米纤维;
步骤2,将所述氨化的聚丙烯腈纳米纤维分散在水溶液中,制得溶液A;将纤维素纳米纤维分散在水溶液中,制得溶液B;将溶液A与溶液B混合、加热、冻干,制得双组分、多重网络纳米纤维气凝胶;
步骤3,取石墨氮化碳,铁源试剂,二氨基对苯二甲酸,步骤2制得的双组分、多重网络纳米纤维气凝胶,加入N,N-二甲基甲酰胺溶剂中,水热反应8~24小时,制得产物。
2.如权利要求1所述的的制备方法,其特征在于,步骤1所述氨化的高分子聚合物纳米纤维的制备方法为:
步骤1.1,以聚丙烯腈高分子聚合物溶液为纺丝液,利用高压静电纺丝技术制备聚丙烯腈纳米纤维;
步骤1.2,将所述聚丙烯腈纳米纤维置于含氨化试剂的水溶液中,调节温度为100~
180℃,加热反应6~24小时。
3.如权利要求2所述的的制备方法,其特征在于,
所述步骤1.1中,纺丝液的质量分数为8%~15%,纺丝电压为10~30kV,纺丝液体流速为0.5~2.0mL/h,收集距离为13~22cm;
所述步骤1.2中,聚丙烯腈纳米纤维的投加量为2g/L~5g/L,氨化试剂的投加量为100g/L~500g/L;
所述氨化试剂为乙二胺、三乙烯二胺、四乙烯五胺,多胺、聚乙烯亚胺中的任意一种。
4.如权利要求1所述的的制备方法,其特征在于,所述步骤2中,加热条件为:置于烘箱中80℃烘0.5~8小时。
5.如权利要求1所述的的制备方法,其特征在于,所述步骤2中,溶液A中氨化的聚丙烯腈纳米纤维与水的质量体积比为5g/L~20g/L,溶液B中质量分数为5%的纤维素纳米纤维溶液与水的体积比为1:5~1:20,溶液A与溶液B的混合体积比为1:1。
6.如权利要求1所述的的制备方法,其特征在于,步骤3中,所述石墨氮化碳的制备方法为:将三聚氰胺在400~550℃条件下,煅烧2~6小时。
7.如权利要求1所述的的制备方法,其特征在于,所述步骤3中,铁源试剂为硝酸铁、氯化铁、硫酸铁中的任意一种。
8.如权利要求1所述的的制备方法,其特征在于,所述步骤3中,石墨氮化碳的投加量为1~5g/L,铁源试剂的投加量为2~10g/L,铁源试剂与二氨基对苯二甲酸的质量比为1:1~1:5,纳米纤维气凝胶的投加量为0.5~2g/L。
9.如权利要求1所述的的制备方法,其特征在于,所述步骤3中,水热反应温度为120~180℃。
10.如权利要求1-9中任一项所述的双组分、多重网络纳米纤维气凝胶负载异质结光催化剂在环境污染处理和能源转化方面的应用。
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Citations (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN104446304A (zh) * | 2014-11-13 | 2015-03-25 | 向军辉 | 多尺度多重网络复合结构的气凝胶复合材料及其制备方法 |
CN104722335A (zh) * | 2015-01-30 | 2015-06-24 | 湖南大学 | 石墨型氮化碳-金属有机框架复合光催化剂及其制备方法和应用 |
CN104785129A (zh) * | 2015-03-31 | 2015-07-22 | 浙江工业大学 | 一种氨化中空纤维膜基底及其用于制备金属有机骨架膜的应用 |
CN104911901A (zh) * | 2014-03-12 | 2015-09-16 | 引领科技无锡有限公司 | 一种静电纺气凝胶复合纳米纤维膜及其制备方法 |
CN109012607A (zh) * | 2018-08-10 | 2018-12-18 | 南通寰宇博新化工环保科技有限公司 | 一种纳米复合材料及其制备方法 |
Family Cites Families (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US20060264132A1 (en) * | 2005-05-21 | 2006-11-23 | Leeser Daniel L | High performance aerogel composites |
CN103285920B (zh) * | 2013-05-27 | 2015-04-08 | 东华大学 | 一种三维纤维基气凝胶催化剂载体及其制备方法 |
CN104611779B (zh) * | 2015-02-11 | 2017-03-01 | 广州金发碳纤维新材料发展有限公司 | 一种聚丙烯腈纺丝原液的氨化方法及其装置 |
-
2019
- 2019-01-25 CN CN201910072377.0A patent/CN109622041B/zh active Active
-
2020
- 2020-01-21 US US16/748,720 patent/US11413608B2/en active Active
Patent Citations (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN104911901A (zh) * | 2014-03-12 | 2015-09-16 | 引领科技无锡有限公司 | 一种静电纺气凝胶复合纳米纤维膜及其制备方法 |
CN104446304A (zh) * | 2014-11-13 | 2015-03-25 | 向军辉 | 多尺度多重网络复合结构的气凝胶复合材料及其制备方法 |
CN104722335A (zh) * | 2015-01-30 | 2015-06-24 | 湖南大学 | 石墨型氮化碳-金属有机框架复合光催化剂及其制备方法和应用 |
CN104785129A (zh) * | 2015-03-31 | 2015-07-22 | 浙江工业大学 | 一种氨化中空纤维膜基底及其用于制备金属有机骨架膜的应用 |
CN109012607A (zh) * | 2018-08-10 | 2018-12-18 | 南通寰宇博新化工环保科技有限公司 | 一种纳米复合材料及其制备方法 |
Non-Patent Citations (1)
Title |
---|
WENYUAN HUANG,ET AL: "Metal organic framework g-C3N4/MIL-53(Fe) heterojunctions with enhanced photocatalytic activity for Cr(VI) reduction under visible light", 《APPLIED SURFACE SCIENCE》 * |
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