Protic‐Salt‐Derived Nitrogen/Sulfur‐Codoped Mesoporous Carbon for the Oxygen Reduction Reaction and Supercapacitors

Abstract

Nitrogen/sulfur-co-doped mesoporous carbon (Phen-HS) was obtained through direct carbonization of a single protic salt, that is, 1,10-phenanthrolinium dibisulfate ([Phen][2 HSO4 ]), in the presence of a colloidal silica template without the use of additional acid or metal catalysts for prepolymerization prior to carbonization. Phen-HS was prepared in a relatively high yield (30.0 %) and has a large surface area (1161 m(2) g(-1) ), large pore volume (2.490 cm(3) g(-1) ), large mesopores (≈12 nm), narrow pore-size distribution (7-16 nm), and high nitrogen (7.5 at %) and sulfur (1.3 at %) contents. The surface area/pore-size distribution is much higher/narrower than that of most reported carbon materials obtained from traditional precursors by using the same template. Phen-HS was directly used as an electrocatalyst for the oxygen reduction reaction (ORR) and as an electrode material for supercapacitors. As an efficient metal-free catalyst, Phen-HS exhibited good electrocatalytic activity toward the ORR in a 0.1 M KOH aqueous solution, which is comparable to the activity of a commercial Pt/C catalyst. Electrochemical measurements for Phen-HS used in a double-layer capacitor showed high specific capacitances of 160 and 140 F g(-1) in 1 M H2 SO4 and 6 M KOH, respectively, with good rate capabilities and high cycling stabilities.

Redox-active triazatruxene-based conjugated microporous polymers for high-performance supercapacitors

“…Specifically, when the nitrogen content increases, the specific capacitance of TAT-CMP-2 at a current density of 1.0 A g –1 increases by nearly 30%. Notably, the remarkable specific capacitance of TAT-CMP-2 is even superior to those of most previously reported porous materials with larger surface areas (Table S1†), such as two-dimensional covalent organic frameworks (48 F g –1 at 0.1 A g –1 , S BET = 1124 m 2 g –1 ), 49 defect-engineered carbon nanotubes ( C = 98 F g –1 at 1 A g –1 , S BET = 988 m 2 g –1 ), 38 nitrogen-doped hierarchical porous carbon nanosheets ( C = 128 F g –1 at 0.1 A g –1 , S BET = 1735 m 2 g –1 ), 39 nitrogen-doped carbon nanoparticles ( C = 84 F g –1 at 1 A g –1 , S BET = 365.3 m 2 g –1 ), 40 sulfur and nitrogen dual-doped porous carbon materials ( C = 129 F g –1 at 10 A g –1 , S BET = 655.4 m 2 g –1 ), 50 nitrogen/sulfur co-doped mesoporous carbon ( C = 160 F g –1 at 1 A g –1 , S BET = 1161 m 2 g –1 ), 51 and copolymer-templated nitrogen-enriched porous carbons ( C = 166 F g –1 at 0.1 A g –1 , S BET = 500 m 2 g –1 ). 52 …”

Design and Materialization of Ionic Liquids Based on an Understanding of Their Fundamental Properties

“…[166][167][168][169][170][171][172][173] Instead of using traditional polymer precursors and complex procedures to prepare N-doped carbons, easily prepared and widely obtainable nitrogencontaining protic ILs/protic salts are used as novel small molecule precursors for the preparation of carbon materials via direct carbonization, without any other treatment (Fig. 14).…”

“…166,167 Resulting from a detailed investigation of the relationship between the precursor structures and the resulting carbon materials, 167 it has become possible to prepare N-doped carbons with controllable N content, 168 and high surface areas with controllable pore structures with or without the use of hard templates. 171 The resulting N-doped carbons exhibit very interesting properties, such as high O 2 reduction activity, 170,172 high CO 2 adsorption capability, 171,173 and high electric double layer capacitance. 170 These low-cost and versatile precursors are promising building blocks for new carbon materials.…”

“…171 The resulting N-doped carbons exhibit very interesting properties, such as high O 2 reduction activity, 170,172 high CO 2 adsorption capability, 171,173 and high electric double layer capacitance. 170 These low-cost and versatile precursors are promising building blocks for new carbon materials.…”

One-step, template-free synthesis of highly porous nitrogen/sulfur-codoped carbons from a single protic salt and their application to CO2 capture

“…The obtained heteroatom-doped, porous carbons have been intensively explored as either electrocatalysts and/or electrode materials for energy storage and conversion. 27 In addition, it is well known that highly porous carbons (surface area > 1000 m 2 /g) are generally obtained via the templating carbonization of organic precursors 28,29 or physical (CO 2 ) 30,31 or chemical (KOH [32][33][34] or ZnCl 2 35 ) activation of the as-synthesized carbons. 26 The former method is highly desirable not only because it can simplify the entire process but also because it allows a homogeneous distribution of N atoms throughout the carbon material.…”