CN114956936A - 一种酞菁铁量子点光催化制备甲烷的方法 - Google Patents
一种酞菁铁量子点光催化制备甲烷的方法 Download PDFInfo
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Abstract
本发明属于能源材料及光催化技术领域,提供了一种酞菁铁量子点光催化制备甲烷的方法。本发明所制备的酞菁铁量子点在水中具有更好的分散性和更大的比表面积,丰富的活性位点可以形成电荷分离态从而抑制电子‑空穴的复合,酞菁铁量子点的量子限域效应让材料拥有更大的有效带隙,增加光催化还原二氧化碳成甲烷的活性。对比酞菁铁粉末,酞菁铁量子点具有更高的催化活性。
Description
技术领域
本发明属于能源材料及光催化技术领域,具体涉及以酞菁铁作为原料,通过至上而下的化学氧化法和多次分离过程制成酞菁铁量子点光催化剂光还原二氧化碳成甲烷的方法。
背景技术
自19世纪工业革命以来,化石能源得到广泛地开发和消耗,造成了很多的环境和能源问题,比如温室效应。面对如此严峻的挑战,科学家们发现太阳能是一个取之不尽,用之不竭且绿色环保的资源,而且二氧化碳是地球上含量最多的温室气体,如果能把这两个资源加以利用,利用太阳能将二氧化碳还原成对人类有用的资源,就可以达到一举两得的目的。
目前制备甲烷的方法有煤催化气化制甲烷,美国Exxon公司对煤制甲烷进行了大量的研究,美国专利US4318712公开了煤制甲烷的整个工作流程,这种方法首先需要消耗掉煤这种能源,同时要求控制炉内高温和需要高温蒸汽、高反应压力,这是对环境不友好和对自生安全存在威胁的。CN105642287A公开了一种甲烷化催化剂制备方法以及由氢气和一氧化碳甲烷化制甲烷的方法,以镍和铝锆柱撑蒙脱石载体,镍负载在铝锆柱撑蒙脱石载体上。该催化剂虽然结构稳定性好和高的甲烷选择性,但是催化剂组成复杂,需要用到贵金属,不利于工业化。CN110066669A公开了一种由生物质制备甲烷的方法,生物质包括木质纤维素、水生材料如藻类等和动物副产品和废料,虽然利用生物质可以达到废物利用和环境友好的目的,但是该方法要用到复杂的反应容器,操作过于复杂。CN101391218A公开了一种适用于焦炉气甲烷化的催化剂,以Al2O3为载体,Ni为主要活性组分,MgO为助剂。Al2O3与助剂MgO按一定比例混合,高温煅烧后形成镁铝尖晶石的载体结构;再用浸渍法引入活性成分。该催化剂具有强度高、低温活性良好等优点,但形成的结构所需的焙烧温度高达1000℃,易造成载体烧结。
基于上述分析,本发明提出以酞菁铁量子点作为光催化剂制备甲烷。我们提出该制备策略主要是基于以下考量:首先利用太阳光,绿色环保且符合可持续发展的理念;酞菁铁量子点不仅具有酞菁铁的优点,即廉价易得,分子结构确定且简单,良好的光稳定性,热稳定性和化学稳定性,在可见光区域有比较宽的响应光谱和吸收强度,还同时具有量子点的优点,即分散性好,高的比表面积,电子和空穴迁移速度快,禁带宽度增加等优点,是理想的制备甲烷的催化剂。反应发生在常温常压下,不需要额外消耗能量来创造高温高压的条件。
发明内容
一种酞菁铁量子点光催化制备甲烷的方法。以酞菁铁为原料,过氧化氢为氧化剂,通过化学氧化法制成了酞菁铁量子点光催化剂。
本发明的技术方案:
一种酞菁铁量子点光催化制备甲烷的方法,包括如下步骤:
将酞菁铁量子点、碱性物质、水按照质量比为1:5:80混匀,在CO2存在和温度为10-60℃条件下,光照催化1-10h得到甲烷。
所述的碱性物质为氢氧化钠、碳酸钠、碳酸氢钠一种或两种以上组合。
光照的光源为装有420nm滤光片的300W氙灯,光照的温度为20-30℃,时间为2-4h。
所述二氧化碳替换为碳酸钠、碳酸氢钠中的至少一种。
所述的酞菁铁量子点的制备方法如下:
(1)制备酞菁铁量子点光催化剂前驱体;将酞菁铁粉末分散在过氧化氢溶液中,得到混合液A;其中,酞菁铁粉末与过氧化氢的摩尔质量比为1:5;
(2)将步骤(1)得到的混合液A置于超声波清洗机中,氧化时间为1-30min,将氧化后的溶液抽滤后,取滤液置于离心机中,离心时间为15-30min,转速为8000-10000r/min,离心次数为1-3次,得到上层清液A;
(3)将步骤(2)得到的上层清液A置于电热恒温鼓风干燥箱中干燥,干燥温度为60-100℃,干燥时间为1-8h,得到酞菁铁量子点。
一种酞菁铁量子点光催化剂制备甲烷由以上制备方法得到,在光催化还原二氧化碳成甲烷的反应中,酞菁铁量子点具有比酞菁铁更好的催化性能。
本发明的有益效果:
1)本发明所制备的酞菁铁量子点比酞菁铁在水中具有更好的分散性,比表面积增加,进一步促进光催化还原二氧化碳成甲烷反应。
2)酞菁铁量子点丰富的活性位点可以形成电荷分离态从未抑制电子-空穴的复合。
3)酞菁铁量子点的量子限域效应让量子点材料拥有更大的有效带隙,更容易发生氧化还原反应
4)酞菁铁的光稳定性、热稳定性和化学稳定性好,来源广、成本低廉,量子点制备工艺简单且绿色无污染。
附图说明
图1是实施例中气相色谱检测结果。
图2是实施例中质谱检测结果。
图3是实施例中使用不同酸碱度进行光催化实验的催化性能图。
图4是实施例中不同酸碱度下酞菁铁量子点的粒径分布图。
具体实施方式
以下结合附图和技术方案,进一步说明本发明的具体实施方式。
实施例1
将1g酞菁铁分散在50mL浓度为30%过氧化氢溶液中,利用搅拌子进行搅拌得到混合液A,将混合液放入超声清洗机中超声15min,将超声后的溶液进行抽滤,将滤液放入离心机中,离心时间为15min,转速为8000r/min,离心2次,得到上层清液A,将上层清液A放入电热恒温鼓风干燥箱中干燥,干燥温度为60℃,干燥时间为4h,得到酞菁铁量子点,取0.1g酞菁铁量子点加入到80mL去离子水中分散,使用碳酸氢钠调整酸碱度使其pH=5,使用该分散体系进行光催化还原二氧化碳性能测试,单位质量的酞菁铁量子点催化剂在单位时间内通过光催化还原二氧化碳得到甲烷的光催化性能为46.127μmol g-1h-1。
表1不同pH值下甲烷产量
实施例2
将1g酞菁铁分散在50mL浓度为30%过氧化氢溶液中,利用搅拌子进行搅拌得到混合液A,将混合液放入超声清洗机中超声5min,将超声后的溶液进行抽滤,将滤液放入离心机中,离心时间为15min,转速为8000r/min,离心2次,得到上层清液A,将上层清液A放入电热恒温鼓风干燥箱中干燥,干燥温度为60℃,干燥时间为4h,得到酞菁铁量子点,取0.1g酞菁铁量子点加入到80mL去离子水中分散,使用碳酸钠调整酸碱度使其pH=11,使用该分散体系进行光催化还原二氧化碳性能测试,单位质量的酞菁铁量子点催化剂在单位时间内通过光催化还原二氧化碳得到甲烷的光催化性能为17.579μmol g-1h-1。
表2不同氧化时间下甲烷的产量
实施例3
将1g酞菁铁分散在50mL浓度为30%的过氧化氢溶液中,利用搅拌子进行搅拌得到混合液A,将混合液放入超声清洗机中超声氧化15min,将超声后的溶液进行抽滤,将滤液放入离心机中,离心时间为15min,转速为8000r/min,离心2次,得到上层清液A,将上层清液A放入电热恒温鼓风干燥箱中干燥,干燥温度为60℃,干燥时间为4h,得到酞菁铁量子点,取0.1g酞菁铁量子点加入到80mL去离子水中分散,使用碳酸钠调整酸碱度使其pH=11,使用该分散体系进行光催化还原二氧化碳性能测试,单位质量的酞菁铁量子点催化剂在单位时间内通过光催化还原二氧化碳得到甲烷的光催化性能为8.086μmol g-1h-1。
表3不同过氧化氢浓度下的甲烷产量
以上所述,仅为本发明较佳的具体实施方式,但本发明的保护范围并不局限于此,任何熟悉本技术领域的技术人员在本发明揭露的技术范围内,根据本发明的技术方案及其发明构思加以等同替换或改变,都应涵盖在本发明的保护范围之内。
Claims (10)
1.一种酞菁铁量子点光催化制备甲烷的方法,其特征在于,包括如下步骤:
将酞菁铁量子点、碱性物质、水按照质量比为1:5:80混匀,在CO2存在和温度为10-60℃条件下,光照催化1-10h得到甲烷。
2.根据权利要求1所述的酞菁铁量子点光催化制备甲烷的方法,其特征在于,所述的碱性物质为氢氧化钠、碳酸钠、碳酸氢钠一种或两种以上组合。
3.根据权利要求1或2所述的酞菁铁量子点光催化制备甲烷的方法,其特征在于,光照的光源为装有420nm滤光片的300W氙灯。
4.根据权利要求1或2所述的酞菁铁量子点光催化制备甲烷的方法,其特征在于,光照的温度为20-30℃,时间为2-4h。
5.根据权利要求3所述的酞菁铁量子点光催化制备甲烷的方法,其特征在于,光照的温度为20-30℃,时间为2-4h。
6.根据权利要求1、2或5所述的酞菁铁量子点光催化制备甲烷的方法,其特征在于,所述二氧化碳替换为碳酸钠、碳酸氢钠中的至少一种。
7.根据权利要求3所述的酞菁铁量子点光催化制备甲烷的方法,其特征在于,所述二氧化碳替换为碳酸钠、碳酸氢钠中的至少一种。
8.根据权利要求4所述的酞菁铁量子点光催化制备甲烷的方法,其特征在于,所述二氧化碳替换为碳酸钠、碳酸氢钠中的至少一种。
9.根据权利要求1、2、5、7或8所述的酞菁铁量子点光催化制备甲烷的方法,其特征在于,所述的酞菁铁量子点的制备方法如下:
(1)制备酞菁铁量子点光催化剂前驱体;将酞菁铁粉末分散在过氧化氢溶液中,得到混合液A;其中,酞菁铁粉末与过氧化氢的摩尔质量比为1:5;
(2)将步骤(1)得到的混合液A置于超声波清洗机中,氧化时间为1-30min,将氧化后的溶液抽滤后,取滤液置于离心机中,离心时间为15-30min,转速为8000-10000r/min,离心次数为1-3次,得到上层清液A;
(3)将步骤(2)得到的上层清液A置于电热恒温鼓风干燥箱中干燥,干燥温度为60-100℃,干燥时间为1-8h,得到酞菁铁量子点。
10.根据权利要求6所述的酞菁铁量子点光催化制备甲烷的方法,其特征在于,所述的酞菁铁量子点的制备方法如下:
(1)制备酞菁铁量子点光催化剂前驱体;将酞菁铁粉末分散在过氧化氢溶液中,得到混合液A;其中,酞菁铁粉末与过氧化氢的摩尔质量比为1:5;
(2)将步骤(1)得到的混合液A置于超声波清洗机中,氧化时间为1-30min,将氧化后的溶液抽滤后,取滤液置于离心机中,离心时间为15-30min,转速为8000-10000r/min,离心次数为1-3次,得到上层清液A;
(3)将步骤(2)得到的上层清液A置于电热恒温鼓风干燥箱中干燥,干燥温度为60-100℃,干燥时间为1-8h,得到酞菁铁量子点。
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