可回收再生NiO/NaBr催化剂蒸汽重整甲醛制氢  

Hydrogen production from formaldehyde steam reforming using recyclable NiO/NaBr catalyst

作　　者：王忠华[1] 储林 葛展志 丁妍 刘优林 沈岳松[2] WANG Zhonghua;CHU Lin;GE Zhanzhi;DING Yan;LIU Youlin;SHEN Yuesong(Jiangsu Sopo(Group)Co.,Ltd.,Zhenjiang 212006,China;College of Materials Science and Engineering,Nanjing Tech University,Nanjing 211816,China)

机构地区：[1]江苏索普(集团)有限公司,江苏镇江212006 [2]南京工业大学材料科学与工程学院,江苏南京211816

出　　处：《能源环境保护》2022年第4期26-36,共11页Energy Environmental Protection

基　　金：国家自然科学基金(51772149);江苏省重点研发计划(BE2021713);江苏省“六大人才高峰”节能环保产业项目(JNHB-044);江苏省青蓝工程;江苏省高校优势学科项目。

摘　　要：采用超临界水热合成法制备了系列可循环回收再生的NiO/NaBr催化剂,用于蒸汽重整甲醛制氢,并结合XRD、N_(2)吸附/脱附、SEM、XPS、H_(2)-TPR、in situ DRIFTS等表征技术,分析了NiO/NaBr催化剂的物相结构、比表面积、微观形貌、元素价态、氧化还原性质及蒸汽重整反应瞬态。结果表明:负载量为1%~5%的NiO/NaBr催化剂均能高效蒸汽重整制氢,2%的NiO/NaBr在450℃时表现出最佳的制氢选择性(104%),甲醛转化率接近100%,一次再生后的催化剂制氢性能可恢复到新鲜水平;NiO/NaBr催化剂表面结构密实,表面积较小(<1 m^(2)·g^(-1)),突破了小比表面催化剂难以获得高质量活性的局限;NiO/NaBr催化剂蒸汽重整甲醛为表面快速反应过程,NiO在此制氢过程中被还原为Ni,并不影响催化活性;NaBr不仅吸附甲醛并形成聚甲醛,还能使催化剂保持较好的低温氧化还原性质及制氢性能。A series of recyclable NiO/NaBr catalysts were prepared by supercritical hydrothermal synthesis for hydrogen production from formaldehyde steam reforming.Combined with XRD,N_(2)adsorption/desorption,SEM,XPS,H_(2)-TPR,in situ DRIFTS and other characterization techniques,the phase structure,specific surface area,microstructure,element valence,redox properties and steam reforming reaction transient of NiO/NaBr catalysts were analyzed.Results showed that 1%~5%NiO/NaBr catalysts efficiently produced hydrogen.2%NiO/NaBr showed the best hydrogen selectivity about 104%at 450℃,and its formaldehyde conversion was close to 100%.The hydrogen production performance after one-time regeneration could return to the fresh level.The NiO/NaBr catalyst had dense surface structure and small surface area(<1 m^(2)·g^(-1)),which broke the limitation that small-surface-area catalyst was difficult to obtain high catalytic activity.The steam reforming of formaldehyde was a surface rapid reaction process.NiO was reduced to Ni without affecting the catalytic activity.NaBr could not only adsorb formaldehyde and form polyformaldehyde,but also help the catalytic maintain great low temperature redox properties and hydrogen production performance.

关 键 词：甲醛 制氢 蒸汽重整 NiO/NaBr催化剂 可回收再生 

分 类 号：X701[环境科学与工程—环境工程]