Synthesis of an ordered porous carbon with the dual nitrogen-doped interfaces and its ORR catalysis performance
Synthesis of an ordered porous carbon with the dual nitrogen-doped interfaces and its ORR catalysis performance
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DOI：
10.1016/j.cclet.2020.11.035
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发表时间：
2020-11
影响因子：
9.1
通讯作者：
Hongwei Zhao;Yan-qiu Zhang;Lixiang Li;Xin Geng;Haiming Yang;Weimin Zhou;Chengguo Sun;B. An
中科院分区：
文献类型：
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作者：
Hongwei Zhao;Yan-qiu Zhang;Lixiang Li;Xin Geng;Haiming Yang;Weimin Zhou;Chengguo Sun;B. An
氮掺杂特性和孔结构是开发具有高氧还原反应性能的氮掺杂碳基催化剂的关键因素。本文以硅烷化的SBA-15为模板，采用乙炔和乙腈气相化学气相沉积法，制备了具有双氮掺杂界面的有序多孔碳（OPC）。在750 °C下CVD 4 h制备的优化样品含有两种类型的有序介孔，一种是继承SBA-15孔的有序圆柱形孔，孔宽为4.0 ~ 5.0 nm;另一种是通过刻蚀SBA-15孔壁产生的有序准六方孔，孔宽为3.0 ~ 4.0 nm。这两种类型的孔的孔壁由CVD产生的氮掺杂碳层构成，从而实际上形成了双氮掺杂界面OPC（DN-OPC）。同时，DN-OPC中含有少量的微孔和较大的比表面积（1430 m2/g）。这种双有序孔和双氮掺杂界面不仅有利于质量传递，而且还利用DN-OPC的活性位点进行ORR。因此，作为无金属的ORR催化剂，DN-OPC表现出接近商业Pt/C催化剂的良好活性，以及优异的耐久性和甲醇耐受性。
Both nitrogen-doping feature and pore structure are critical factors for developing nitrogen-doped carbons based catalysts with a high performance toward oxygen reduction reaction (ORR). Herein, a simple one-step CVD of acetylene and acetonitrile vapor method using silanized SBA-15 as a template has been developed to synthesize an ordered porous carbon (OPC) with dual nitrogen-doped interfaces. The optimized sample as prepared with the CVD of 4 h at 750 °C contains two types of ordered mesopores that one type is the ordered cylindrical pores inheriting from the pores of SBA-15 and has a pore width of 4.0∼5.0 nm, the other type is the ordered quasi-hexagonal pores with a width of 3.0∼4.0 nm produced by etching the pore walls of SBA-15. These two types of pores whose pore walls are built by the nitrogen doped carbon layers resulted by the CVD and thus it actually makes the dual nitrogen-doped interfaced OPC (DN-OPC). Meanwhile, DN-OPC contains a few of micropores and a large SSA of 1430 m2/g. This dual-ordered pores and dual nitrogen-doped interfaces cannot only facilitate mass transport but also utilize the active sites of DN-OPC for ORR. Therefore, as metal-free ORR catalyst, DN-OPC exhibits a good activity close to commercial Pt/C catalyst, and an excellent durability and methanol tolerance.