CN113398926A - 一种用于CO2催化加氢制甲醇的Pt/In2O3催化剂及其制备方法 - Google Patents
一种用于CO2催化加氢制甲醇的Pt/In2O3催化剂及其制备方法 Download PDFInfo
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Abstract
本发明公开了一种用于CO2催化加氢制甲醇的Pt/In2O3催化剂及其制备方法，涉及催化剂设计领域。本发明所述Pt/In2O3催化剂由In2O3与Pt(NO3)2在水中共同浸渍后焙烧而得，本发明通过浸渍法，将Pt原子镶嵌在In2O3的晶格里，在CO2加氢过程中，部分带正电荷的Pt物种被还原并烧结，形成Pt纳米粒子，而其他的Pt保持原子分散的带正电荷状态，对H2吸附分解有较好活性；并且有助于产生更多的氧空位，从而激活CO2，促进CO2加氢反应，从而实现更高的催化活性。
Description
技术领域
本发明涉及催化剂设计领域，具体涉及的是一种用于CO2催化加氢制甲醇的Pt/In2O3催化剂及其制备方法。
背景技术
化石燃料的过度消耗引发了人们对环境问题和国家能源安全的担忧，因此，寻求环保可再生的替代燃料的需求越来越高。目前，CO2作为广泛存在的碳源，在化学工业中起着越来越重要的作用，是很有前途的可再生能源之一。对CO2进行催化加氢制备甲醇等高附加值化学产品具有极高的经济价值。
现有技术中，Cu/TiO2催化剂是CO2进行催化加氢制备甲醇等高附加值化学产品的常见化学催化剂，但现有的Cu/TiO2催化剂，虽然在对CO2进行催化加氢制备甲醇等高附加值化学产品的化学反应中表现出了较高的催化活性，但其催化转化率实质上都只有50％左右，因此，除了提升Cu/TiO2催化剂的催化活性，也有必要针对CO2进行催化加氢制备甲醇等高附加值化学产品化学反应开发催化活性更高的催化剂。
除了Cu/TiO2催化剂，Pt负载在传统的活性炭上，针对CO2进行催化加氢制备甲醇等高附加值化学产品化学反应，也能实现一定的催化效果，但催化活性不大，还不如Cu/TiO2催化剂。
发明内容
本发明旨在提供一种用于CO2催化加氢制甲醇的Pt/In2O3催化剂及其制备方法，在针对CO2进行催化加氢制备甲醇等高附加值化学产品化学反应中，用解决现有催化剂催化活性不够高的技术问题。
为实现上述目的，本发明采用的技术方案如下：
一种用于CO2催化加氢制甲醇的Pt/In2O3催化剂，所述Pt/In2O3催化剂由In2O3与Pt(NO3)2在水中共同浸渍后焙烧而得。
一种用于CO2催化加氢制甲醇的Pt/In2O3催化剂的制备方法，包括如下步骤：
(1)制备In2O3；
(2)将In2O3分散于水中，并加入Pt(NO3)2，浸渍20～30h，旋蒸得到固体粉末；
(3)将旋蒸所得固体粉末在350～450℃下焙烧2～4h，即得到Pt/In2O3催化剂。
作为优选地，所述步骤(1)中，In2O3的制备过程为：a.将氨水溶于乙醇得到溶液A；b.将硝酸铟或硝酸铟的水合物溶于乙醇和水的混合溶液中，制得溶液B；c.将A、B溶液混合，并于60-90℃下搅拌2～4h，得到固体沉淀；d.分离得到沉淀并水洗、干燥，得到的固体于400～500℃下焙烧2～4h，即得到In2O3。
进一步地，步骤a、b中，以40ml添加量、质量分数为25～28％的氨水计算，溶液A中含乙醇120ml；溶液B中水合硝酸铟的添加量为14g，水和乙醇体积比为1∶3，乙醇和水共计160ml。
作为优选地，步骤(2)中，以与1g In2O3计算，Pt(NO3)2添加量为0.11g，水的使用量为100ml。
与现有技术相比，本发明具有以下有益效果：
1、本发明通过浸渍法，将Ptn+离子镶嵌在In2O3的晶格里，在CO2加氢过程中，部分带正电荷的Pt物种被还原并烧结，形成Pt纳米粒子，而其他的Pt保持原子分散的带正电荷状态，对H2吸附分解有较好活性；并且有助于产生更多的氧空位，从而激活CO2，促进CO2加氢反应，从而实现更高的催化活性；
2、本发明制备的Pt/In2O3催化剂，所用原料药剂安全易得，用于CO2催化加氢制甲醇，在较低温度以及常压条件下表现出较高的催化反应活性，可用于绿色环保新能源的开发与应用。
3、相当于In2O3的现有制备方法，本发明使用氨水、硝酸铟共沉淀进行制备，制备的In2O3结构更为松散，方便下一步Pt的浸渍，使得Ptn+离子顺利镶嵌在In2O3的晶格里。
附图说明
图1为实施例1制备的Pt/In2O3催化剂透视电镜图；
图2为采用Pt/C与实施例1制备的Pt/In2O3对CO2催化剂催化加氢的个产物收率对比图。
具体实施方式
为了使本领域的技术人员更好地理解本发明的技术方案，下面结合各实施例和附图对本发明作进一步说明，本发明的实现方式包括但不仅限于以下实施例。
本发明提供了一种Pt/In2O3催化剂，所述Pt/In2O3催化剂是由In2O3与Pt(NO3)2在水中共同浸渍后焙烧而得。以下实施例、对照实验结合附图内容进一步说明Pt/In2O3催化剂的制备过程以及产品结构、性能。
实施例1
本实施例提供了Pt/In2O3催化剂的一种制备方法，包括如下步骤：
a)将40mL氨水(25.0-28.0％)与120mL无水乙醇混合，制得溶液A；
b)将14g的In(NO3)3·xH2O溶于40mL水和120mL乙醇的混合物中，制得溶液B；
c)将溶液A与溶于B混合，在80℃下进行2h的搅拌，得到固态沉淀；
d)将沉淀离心分离，用水洗涤三次，在70℃下空气中干燥。随后得到的固体在450℃的空气中煅烧3h，得到In2O3；
e)将0.11g的Pt(NO3)2与1g的In2O3在100mL水中浸渍24h，用旋转蒸发器干燥得到固体粉末；
g)将上述固体粉末在400℃下焙烧2h，得到Pt负载量为2wt％的Pt/In2O3，其结构形貌如图1。
对照实验
以实施例1制备的Pt/In2O3催化剂为实验组，以Pt/C催化剂为对照组，将20mg催化剂装入直径为1cm的直管石英反应器中，加热到240℃进行反应。反应器进口气体流量是100mL/min，气体成分是30％H2，10％CO2和60％的Ar。反应器出口处使用质谱仪对反应后的气体成分进行分析，计算各组分收率，汇总后得到如图2所示的柱状图。
由图二不难得出，相较于Pt/C催化剂，实施例1制备的Pt/In2O3对CO2催化剂在活性和选择性上均有进一步提升。
上述实施例仅为本发明的优选实施方式之一，不应当用于限制本发明的保护范围，但凡在本发明的主体设计思想和精神上作出的毫无实质意义的改动或润色，其所解决的技术问题仍然与本发明一致的，均应当包含在本发明的保护范围之内。
Claims (5)
1.一种用于CO2催化加氢制甲醇的Pt/In2O3催化剂，其特征在于，所述Pt/In2O3催化剂由In2O3与Pt(NO3)2在水中共同浸渍后焙烧而得。
2.一种如权利要求1所述的用于CO2催化加氢制甲醇的Pt/In2O3催化剂的制备方法，其特征在于，包括如下步骤：
(1)制备In2O3；
(2)将In2O3分散于水中，并加入Pt(NO3)2，浸渍20～30h，旋蒸得到固体粉末；
(3)将旋蒸所得固体粉末在350～450℃下焙烧2～4h，即得到Pt/In2O3催化剂。
3.如权利要求2所述的制备方法，其特征在于，所述步骤(1)中，In2O3的制备过程为：
a.将氨水溶于乙醇得到溶液A；
b.将硝酸铟或硝酸铟的水合物溶于乙醇和水的混合溶液中，制得溶液B；
c.将A、B溶液混合，并于60-90℃下搅拌2～4h，得到固体沉淀；
d.分离得到沉淀并水洗、干燥，得到的固体于400～500℃下焙烧2～4h，即得到In2O3。
4.如权利要求3所述的制备方法，其特征在于，步骤a、b中，以40ml添加量、质量分数为25～28％的氨水计算，溶液A中含乙醇120ml；溶液B中水合硝酸铟的添加量为14g，水和乙醇体积比为1∶3，乙醇和水共计160ml。
5.如权利要求2所述的制备方法，其特征在于，步骤(2)中，以与1g In2O3计算，Pt(NO3)2添加量为0.11g，水的使用量为100ml。
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Cited By (4)
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| CN114160198A (zh) * | 2021-12-16 | 2022-03-11 | 中国船舶重工集团公司第七一九研究所 | 用于CO2催化加氢制甲醇的Pt/POP催化剂及其制备方法 |
| CN114405505A (zh) * | 2022-01-25 | 2022-04-29 | 上海工程技术大学 | 一种铂修饰铟基氧化物催化剂及其制备方法和应用 |
| CN114703659A (zh) * | 2022-03-14 | 2022-07-05 | 陕西师范大学 | Pt/In2O3-x复合纳米纤维材料及其制备方法和应用 |
| CN115945191A (zh) * | 2023-02-10 | 2023-04-11 | 江南大学 | 一种氧化铟负载的单原子催化剂及其制备方法与应用 |
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