CN1322266C - 一种储氢器 - Google Patents
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Abstract
一种储氢器，其特征在于：该储氢器中装入颗粒状的储氢材料与不吸氢的金属纤维和/或其合金纤维的混合物，且混合物中不吸氢的金属纤维和/或其合金纤维的重量为储氢材料重量的1～10%。同现有技术比较，本发明具有以下突出的优点：1)装入储氢器内的混合物中的纤维有足够大的表面积，能有效防止储氢材料及其氢化物粉末流动形成堆积；2)在储氢材料中加少量不吸氢的金属纤维和/或其合金纤维，即能有效提高储氢材料及其氢化物粉末的传热性能；3)本储氢器中的储氢材料不必预先进行镀铜、压块、中毒、烧结、反复吸放氢循环等处理或加工，也不用添加有机溶剂或造孔剂，因此具有廉价、高效、长期运行安全可靠的特点。
Description
技术领域
本发明涉及一种氢气的储存、输送及压缩技术，特别涉及一种储氢器。
背景技术
氢是重要的工业原料，也是一种理想的洁净燃料和未来的重要二次能源。目前实际应用的氢气储存与输送的方式主要有三种，即高压容器(钢瓶)、液氢储罐(低温杜瓦瓶)及金属氢化物储氢器。用金属氢化物储氢器储存、输送氢气的突出优点是安全性好，单位重量储氢密度远高于高压容器和液氢储罐。由于金属氢化物本身具有多种功能：如进行氨气提纯、分离与回收；作为氢气压缩以及能量转换系统(蓄热、制冷、空调、取暖、热机)的介质等，因此其技术发展倍受关注。尤其是以氢作为燃料的燃料电池在汽车、助动车、摩托车、通讯、电脑、摄像机、电动工具以及军事装置等应用领域的逐步推开，作为随车或移动式储氢载体(氢燃料箱)具有很大的市场前景。
把储氢材料放入一个带阀门的容器内就可构成一个储氢器。容器内的储氢材料在吸、放氢过程中存在热效应，其热效应值随储氢材料不同而异，通常为25～75千焦耳/摩尔，由此可见要维持储氢器内储氢材料的吸、放氢的顺利进行，就必须相应地向储氢器输入热量或从储氢器输出热量。储氢材料一旦吸氢和转变为氢化物时，体积随即膨胀，体积膨胀率为14～25％，并粉化为微米级的细粉，反复进行吸放氢循环，粉化则持续进行，由于金属氢化物本身的导热性很差，相当于玻璃、砂石的导热性，导致及时向储氢器内输入热量或从储氢器输出热量变得相当困难，使得吸氢时储氢材料温升急剧升高，或放氢时储氢材料温度急剧下降，造成吸放氢速度缓慢甚至停止；此外储氢材料细粉或氢化物细粉在吸放氢操作过程中，因受氢气流的驱动会在储氢器内某一部位形成过量堆积，导致容器变形或胀破。所以改善储氢器内粉体的传热性能和防止粉体在某一部位的过量堆积，成为需要优先解决的技术问题。
有人采用不吸氢的金属粉末，如铝粉、铜粉、镍粉与储氢材料粉末混合压制成块状，再经烧结后使用，结果实验失败了，原因是烧结后的压块没有足够的空隙，不能为材料吸氢膨胀提供所需的空间；随后对上述方案进行了改进，对储氢材料预先进行数次至数十次吸放氢操作，然后在吸氢状态下通入SO2，使合金中毒以保持体积膨胀状态，再进行压块，此压块经1000次吸放氢循环而不碎裂。此方案的缺陷是：制备过程复杂，而且储氢材料经中毒和烧结，使储氢容量降低15％以上，见参考文献[1][2]。
文献[3]报导了另一种技术，即将储氢材料与铝粉及造孔剂构成混合料，并压制成块状，再经60～80℃烘烤去除大部分造孔剂后，在真空下烧结定型，如此制成的压块经1000次循环吸放氢而不发生碎裂。该方案省略了预先多次吸放氢循环和“中毒”操作，工序简化，成本降低，但储氢容量仍降低15％左右。文献[4]提供了一种镀铜一压块的制备方案，储氢合金粉经敏化处理后放入镀铜液中镀铜，镀覆后的储氢合金粉末在真空或者氩气中加热释放出镀铜过程中合金粉吸收的氢气，然后在100～1000MPa压力下压制成块状；镀铜之前，储氢合金粉必须预先进行10次以上的吸放氢循环，以确保合金粉化充分和粒度稳定，避免镀铜后的合金粉因吸氢膨胀而破坏镀层，显然该方案增加了10次以上的吸放氢操作和镀铜工序，成本提高，且镀覆的铜层不能吸氢，储氢容量也下降10％以上。
美国布鲁克海文国家实验室提出了向盛装储氢材料的容器内注入正十一烷、正辛烷或者硅油之类有机溶剂，使有机溶剂与储氢材料颗粒形成悬浮液，见参考文献[5][6]。储氢材料在这类有机溶剂中照样能进行可逆吸放氢反应，传热性能得到改善，容器也不会胀坏，但由于加入了大量不会吸氢的有机溶剂，使储氢器的单位重量和单位体积的储氢密度均大幅度降低。
发明内容
本发明的目的在于提供一种储氢器，将储氢材料和不吸氢的金属纤维或者其合金纤维的混合物直接装入该储氢器内，储氢器内的混合物传热性能良好，反复吸放氢操作不会损坏容器，具有安全、高效、廉价的特点，这种储氢器既适用于固定式的储氢应用场合，也适用于移动式或便携式储存与输送氢气的场合，如氢燃料电池、燃氢内燃机车辆的氢燃料箱等。
一种储氢器，包括壳体，阀门，其特征在于：该储氢器中装入颗粒状的储氢材料与不吸氢的金属纤维和/或其合金纤维的混合物，且混合物中不吸氢的金属纤维和/或其合金纤维的重量为储氢材料重量的1～10％；混合物中的不吸氢金属纤维或合金纤维是铝及其合金的纤维、铜及其合金的纤维、镍及其合金的纤维中的一种，或者是几种；不吸氢的金属纤维或其合金纤维，其长度为3～20mm，断面尺寸不大于2平方毫米。上述混合物中的储氢材料，可选用稀土系储氢合金，钛系储氢合金，锆系储氢合金，镁、钙、碱土金属及其储氢合金，或者是上述金属或合金的氢化物；混合物中的不吸氢的金属纤维或其合金纤维的导热率高，如Al、Cu、Ni的导热率分别为222、394、92Jm-1s-1k-1，而TiFe合金粉末和LaNi5合金粉末的导热率仅为1.49和1.32Jm-1s-1k-1，前者的导热率比后者导热率大60～300倍，这些纤维分布于储氢材料颗粒之间，有效地提高储氢材料颗粒以及整个混合物料层的传热性能；而且这类纤维具有三维外形，表面粗糙，如图1所示。与添加同类金属或合金粉比较，添加这类纤维组成的混合物的堆比重更小，表明混合物存在更多的空隙，亦即能为储氢材料吸氢膨胀提供更大的退让空间；而且这类纤维能更好和更均匀地构成一种网络骨架，从而更有效的起到阻止储氢材料粉末的流动与堆积的作用。这类纤维可采用上述不吸氢的金属或其合金切削下来的切屑。
同现有技术比较，本发明的突出优点是：1)将颗粒状的储氢材料与不吸氢的金属纤维和/或其合金纤维混合物装入储氢器中，该混合物中的纤维有足够大的表面积，能有效防止储氢材料及其氢化物粉末流动形成堆积；2)在储氢材料中加少量不吸氢的金属纤维和/或其合金纤维，即能有效提高储氢材料及其氢化物粉末的传热性能，混合物中纤维含量越少，混合物的总储氢量降低就越少；3)本储氢器中的储氢材料不必预先进行镀铜、压块、中毒、烧结、反复吸放氢循环等处理或加工，也不用添加有机溶剂或造孔剂，因此具有廉价、高效、长期运行安全可靠的特点。
附图说明
图1为一种铝合金纤维的外形图。
具体实施方式
实施例1：
储氢材料为稀土系储氢合金MmNi4.5Mn0.5，式中Mm为混合稀土金属，先将MmNi4.5Mn0.5破碎形成粒度不大于3mm的颗粒；铝纤维长度为3mm，其断面尺寸为0.5平方毫米，铝纤维的重量为上述储氢材料重量的1.0％，两者混匀后装入带有壳体及阀门的容器即构成储氢器，混合物的堆比重为每立方厘米3.6克。对储氢器排气至133Pa后导入纯度为99.99％、压力为4.0MPa氢气，储氢器内的储氢合金开始吸氢，并逐渐转化为氢化物，吸氢饱和后完全转化为氢化物粉末，首次活化完成，该储氢器即可投入使用。实测结果：混合物的重量储氢密度为1.4％，混合物的导热率为5.2Jm-1s-1k-1，在室温、压力为4.0MPa下吸氢和对0.1MPa大气放氢的1000次反复吸放氢循环操作后，储氢器未出现膨胀或任何损坏。
实施例2：
储氢材料为钛系TiFe0.85Mn0.15合金，不吸氢的金属纤维为黄铜纤维，其长度为11mm，断面尺寸为1.2平方毫米，黄铜纤维重量为储氢合金的重量的5％，两者混匀后装入储氢器，混合物堆比重为3.0克/立方厘米。活化过程与实施例1相同。实测结果：混合材料的重量储氢密度为1.7％，在室温下经1000次反复吸放氢操作，该储氢器完好无损。
实施例3：
选用镁系合金Mg2Ni作为储氢材料，不吸氢的合金纤维为镍合金纤维，其长度为20mm，断面尺寸为2平方毫米，镍合金纤维的重量为储氢材料重量的10％，Mg2Ni合金破碎成小于5mm的颗粒，两者混匀后装入储氢器，混合物的堆比重为2.2克/立方厘米。活化过程：对储氢器抽空至50Pa，加热升温至300℃，在升温加热过程中继续保持储氢器内的真空度，然后导入纯度为99.99％、压力为3.0MPa氢气，Mg2Ni开始活化，吸氢饱和时活化完成，Mg2Ni转变为Mg2NiH4，氢即储存在合金中。实测结果：混合物的重量储氢密度为3.25％，在300℃下经1000次反复吸放氢操作，储氢器完好无损。
参考文献[1]Proc.Int.Symp，On Hydrides for Energy Storage，Pergamon，Oxford，1978，P417-430
[2]J.of the Less-Common Met，74，1980，P445-448
[3]Z.füer Phys.Chem，164，1989，P1367-1372
[4]J.of the Less-Common Met，107，1985，P105-110
[5]J.of the Less-Common Met，104，1985，P175-190
[6]J.of the Less-Common M
Claims (3)
1.一种储氢器，包括壳体，阀门，其特征在于：该储氢器中装入颗粒状的储氢材料与不吸氢的金属纤维和/或其合金纤维的混合物，且混合物中不吸氢的金属纤维和/或其合金纤维的重量为储氢材料重量的1～10％。
2.根据权利要求1所述的储氢器，其特征在于：混合物中的不吸氢金属纤维或合金纤维是铝及其合金的纤维、铜及其合金的纤维、镍及其合金的纤维中的一种，或者是几种。
3.根据权利要求1和2所述的储氢器，其特征在于：不吸氢的金属纤维或其合金纤维，其长度为3～20mm，断面尺寸不大于2平方毫米。
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| CN100362130C (zh) * | 2005-12-15 | 2008-01-16 | 哈尔滨工程大学 | 一种储氢合金表面化学镀铜的方法 |
| US7946228B2 (en) * | 2008-05-09 | 2011-05-24 | Wendy Gainsborough, legal representative | Self contained non toxic obscurant grenade and self-contained aerosol dispersing grenade |
| US20100061926A1 (en) * | 2008-09-11 | 2010-03-11 | Gm Global Technology Operations, Inc. | Heating systems for hydrogen storage materials |
| FR2939784B1 (fr) * | 2008-12-16 | 2012-02-03 | Centre Nat Rech Scient | Reservoir adiabatique d'hydrure metallique |
| US8418841B2 (en) * | 2010-05-14 | 2013-04-16 | Ford Global Technologies, Llc | Method of enhancing thermal conductivity in hydrogen storage systems |
| CN102432408B (zh) * | 2011-09-19 | 2013-05-01 | 中国科学技术大学 | 氢化钛型储氢乳化炸药 |
| CN102563339B (zh) * | 2011-12-31 | 2015-09-09 | 北京浩运金能科技有限公司 | 一种金属氢化物储氢装置 |
| US9206945B2 (en) * | 2012-02-15 | 2015-12-08 | Ford Global Technologies, Llc | System and method for hydrogen storage |
| CN104100834A (zh) * | 2013-04-03 | 2014-10-15 | 北京浩运金能科技有限公司 | 一种可快速吸放氢的金属氢化物储氢装置 |
| US10386121B2 (en) * | 2013-10-21 | 2019-08-20 | Advanced Cooling Technologies, Inc. | Open-loop thermal management process and system |
| CN106608616B (zh) * | 2015-10-21 | 2020-05-08 | 亚太燃料电池科技股份有限公司 | 储氢组合物及其储氢容器的制造方法 |
| US10024498B2 (en) * | 2015-10-21 | 2018-07-17 | Asia Pacific Fuel Cell Technologies, Ltd. | Hydrogen storage composition, hydrogen storage container and method for producing hydrogen storage container with hydrogen storage composition |
| US11333303B2 (en) | 2015-10-21 | 2022-05-17 | Asia Pacific Fuel Cell Technologies, Ltd. | Hydrogen storage composition, hydrogen storage container and method for producing hydrogen storage container with hydrogen storage composition |
| CN105842230B (zh) * | 2016-03-29 | 2018-06-22 | 中国科学院上海硅酸盐研究所 | 一种用于重金属元素检测的装置及方法 |
| CN105675612A (zh) * | 2016-04-25 | 2016-06-15 | 天津大桥焊材集团有限公司 | 一种扩散氢的分析装置及分析方法 |
| CN109970024B (zh) * | 2019-03-21 | 2022-12-09 | 江苏集萃安泰创明先进能源材料研究院有限公司 | 一种高导热性的储氢材料及其制备方法 |
| CN110788331B (zh) * | 2019-11-07 | 2022-10-11 | 江苏集萃安泰创明先进能源材料研究院有限公司 | 含铜复合储氢合金及其制备方法、复合固态储氢罐及储放氢性能测试方法 |
| CN110788330B (zh) * | 2019-11-07 | 2022-02-11 | 江苏集萃安泰创明先进能源材料研究院有限公司 | 含铝复合储氢合金及其制备方法、复合固态储氢罐及储放氢性能测试方法 |
| CN112694373B (zh) * | 2021-02-05 | 2023-06-16 | 中国科学技术大学 | 一种螺旋空心铝纤维储氢复合炸药及其制备方法 |
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