锰结核氨浸渣脱硫剂净化高温气体中硫化氢作用机理

In industrial hot gases, hydrogen sulfide(H2S) is toxic for catalysts as well as corrosive to most equipments. A novel desulfurized material with high thermalstability and efficiency are needed..In this work, manganese nodules leached residue (MNLR) from the Pacific has been applied to remove H2S at high temperature and found to be effective. A combination of varied mineral characterizations including HR-TEM and H2S on-line monitoring measurement will be performed to investigate the H2S removal mechanism at high temperature. The main objectives of this work are to characterize the synthesis between iron and manganese phases, microsturctual transformation of iron-mananese oxides in MNLR at high temperature. The desulfurization velocity and efficiency will be achieved as well. The variations of high-temperature products will be determined in order to check the effects resulted from chemical compositions of MNLR including iron, manganese and impurity. The extensive investigations of desulfurized product and its regeneration method are also gong to be performed. Mixed iron-manganese spinel oxides in MNLR have been observed. In addition, a correlation between chemical composition, structure, morphology of MNLR and high-temperature desulfurization capacity will be explained in this work..Thus, an exploration in the theory of H2S removal from hot gases by MNLR is performed in this work. It will promote the development of environmental mineralogy and mineral materials.

高温煤气中硫化氢易造成催化剂中毒、管道腐蚀等危害，耐高温的高效脱硫剂有待深入研究。本课题前期研究发现，大洋锰结核氨浸渣煅烧产物在高温下脱除硫化氢具有独特的优势。本项目拟采用高分辨电镜等多种矿物学表征手段，结合气相分子吸收光谱、小型质谱仪等气体在线监测方法，进一步研究氨浸渣高温脱硫作用机理，重点解析：高温下氨浸渣中铁锰各矿物相之间的化合反应过程、矿物相和微结构演化规律；高温还原气氛下氨浸渣脱硫反应速率、脱硫效率的影响因素；氨浸渣中铁、锰及其它杂质组分在脱硫反应中的作用及其对高温衍生结构的制约；脱硫反应产物、脱硫剂的再生方法和条件。阐明氨浸渣在高温脱硫反应过程中铁锰尖晶石产生及其成分、结构、形貌等矿物学特征与脱硫反应的关系。为大洋锰结核氨浸渣应用及高温气体中硫化氢深度净化提供理论支撑，推动环境矿物学和矿物材料的发展。

高温煤气中硫化氢易造成催化剂中毒、管道腐蚀等危害，锌、铁等金属及其氧化物来源丰富、价格低廉，在常温下可作为较好的脱硫材料，但高温下它们的脱硫性能均受到制约。因此，对于耐高温的高效脱硫剂有待深入研究。.本课题研究发现，氨浸渣、铜陵锰矿及叶山褐铁矿等煅烧产物在高温下脱除硫化氢具有独特的优势。故采用多种矿物学表征手段，结合气相分子吸收光谱硫化氢在线监测方法，研究了大洋锰结核氨浸渣等天然锰铁矿物高温脱硫作用机理，重点解析了高温下铁锰各矿物相之间的化合反应过程、矿物相和微结构演化规律；高温还原气氛下氨浸渣等天然矿物脱硫反应速率、脱硫效率的影响因素；脱硫剂中铁、锰及其它杂质组分在脱硫反应中的作用及其对高温衍生结构的制约；脱硫反应产物、脱硫剂的再生方法和条件。.课题研究发现，氨浸渣、铜陵锰矿及叶山褐铁矿等天然矿物经一定热处理反应后产物为Mn(Fe)O，可作为高温脱硫剂；其最佳脱硫反应温度为700 ℃，最佳气速为40 mL/min。其中大洋锰结核氨浸渣煅烧产物脱硫剂初次脱硫容量为126 mgS/g脱硫剂，9次再生后的脱硫容量之和为1233 mgS/g脱硫剂；软锰矿初次脱硫容量为122 mgS/g脱硫剂，9次再生后的脱硫容量之和为1240 mgS/g脱硫剂；叶山褐铁矿脱硫剂初次脱硫容量为162 mgS/g脱硫剂，9次再生后的的脱硫容量之和为1609 mgS/g脱硫剂。同时氨浸渣脱硫剂可再生为方铁锰矿，高温脱硫作用除了Mn(Fe)O与硫化氢的硫化反应外，还存在硫化产物Mn(Fe)S对硫化氢的催化裂解次反应。.本项研究阐明了氨浸渣、铜陵锰矿及叶山褐铁矿等天然锰铁矿物在高温脱硫反应过程中铁锰复合氧化物产生及其成分、结构、形貌等矿物学特征与脱硫反应的关系。为铁锰氧化物矿物应用于高温气体中硫化氢深度净化提供理论支撑，推动环境矿物学和矿物材料的发展。. 本项目已在国际SCI期刊发表论文1篇，接收待刊2篇；在国内核心期刊发表EI收录论文1篇；申请2项国家发明专利，已授权1项，培养硕士研究生2名。