g-C_(3)N_(4)催化石墨化碳质材料的制备及光催化性能研究  

Synthesis and Photocatalytic Performance of Catalytic Graphitization of g-C_(3)N_(4) Carbonaceous Materials

作　　者：李悦[1,2] 王博[1,2,3] 朱晓丽 刘昆[1] LI Yue;WANG Bo;ZHU Xiaoli;LIU Kun(Department of Environmental and Chemical Engineering, Tangshan University, Tangshan 063000, China;State Key Laboratory of Metastable Materials Science and Technology, Yanshan University, Qinhuangdao 066004, China;Key Laboratory of Chemical Environmental Protection and New Film Coating Materials in Tangshan City, Tangshan 063000, China)

机构地区：[1]唐山学院环境与化学工程系,唐山063000 [2]亚稳材料制备技术与科学国家重点实验室(燕山大学),秦皇岛066004 [3]唐山市化工环保与新型薄膜涂层材料重点实验室,唐山063000

出　　处：《人工晶体学报》2021年第11期2156-2163,共8页Journal of Synthetic Crystals

基　　金：亚稳材料制备技术与科学国家重点实验室开放课题(202103);河北省高等学校科学技术研究项目(QN2019316)。

摘　　要：通常采用以氢氧化物作为造孔剂,过渡金属硝酸盐或氯化物作为石墨化催化剂的传统两步法策略制备多孔石墨化碳材料。然而制备过程中多涉及有毒和腐蚀性试剂,且多步骤的过程耗时较长。本文以双氰胺为原料通过热缩聚反应得到g-C_(3)N_(4),采用高铁酸钾为催化剂一步法实现g-C_(3)N_(4)的同步碳化-石墨化,并研究其光催化性能。与传统的两步法相比,该方法耗时少、效率高、无污染。与初始的g-C_(3)N_(4)材料相比,石墨化g-C_(3)N_(4)衍生碳质材料不仅显著改善了可见光的吸收,而且大大增强了光催化活性。研究了不同石墨化温度对g-C_(3)N_(4)衍生碳质材料在可见光下降解甲基橙溶液的影响。700℃下制备的衍生碳质材料的降解率为12.4 mg/g。光电化学测试结果表明,多孔g-C_(3)N_(4)衍生碳质材料的光生载流子密度、电荷分离和光电流(提高了5.4倍)均得到显著提高。因此,该简便、灵活方法为提高g-C_(3)N_(4)衍生碳质材料的吸附和光催化性能提供了一种有前景的、高效的途径。The preparation methods for porous graphitic carbon materials have mostly employed a conventional two-step strategy,in which hydroxides act as the pore-forming agent and transition metal nitrates or chlorides as the graphitization catalyst.However,most of the reagents mentioned above are toxic and corrosive,and multi-step processes are time-consuming.In this work,a one-step strategy to synthesize porous graphitic g-C_(3)N_(4)-derived carbon materials was established,and its photocatalytic performance was studied.The g-C_(3)N_(4) bulks were prepared by conventional thermal polycondensation approach from dicyandiamide.Potassium ferrate(K_(2)FeO_(4))was utilized as both activating agent and catalyst to fulfil the synchronous carbonization and graphitization of g-C_(3)N_(4),this method is less time-demanding,highly efficient and pollution-free,when compared with a conventional two-step strategy.The g-C_(3)N_(4)-derived carbon materials delivers not only significantly improved visible-light absorption but also greatly enhanced photocatalytic activity compared to pristine g-C_(3)N_(4).The effect of g-C_(3)N_(4)-derived carbon materials with different graphitization temperature on the degradation of methyl orange(MO)solution under visible light was studied.The results indicate that the degradation rate of g-C_(3)N_(4)-derived carbon materials prepared at 700℃is 12.4 mg/g.Photoelectrochemical measurements reveal that the porous graphitic samples exhibit improved carrier densities,charge separation,and photocurrent(a 5.4-fold increase)compared to that of the original g-C_(3)N_(4).Consequently,this facile and versatile method could provide a promising and cost-effective approach to improve the absorption and photocatalysis performance of g-C_(3)N_(4)-derived carbonaceous materials.

关 键 词：石墨氮化碳 碳质材料 光催化 高铁酸钾 碳化-石墨化 可见光 甲基橙 

分 类 号：O643.3[理学—物理化学]