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### 石墨碳氮化物衍生的多孔碳网络用于高效氧还原反应 #### 背景与意义氧还原反应（Oxygen Reduction Reaction, ORR）是清洁能源转换策略（如燃料电池和金属-空气电池）中的关键步骤之一[1]。传统上，铂基材料作为ORR的阴极材料广泛被采用，但这类材料存在成本高、稳定性有限及对甲醇耐受性差等问题[1,4-8]。因此，开发低成本、高活性、耐用的ORR材料成为近年来研究的重点[9,10]。 #### 研究背景在寻找替代铂基电催化剂的过程中，过渡金属催化剂和基于碳的纳米材料受到了广泛关注[5,11-16]。特别是作为无金属电催化剂，基于碳的纳米材料因其良好的耐用性、不含贵金属以及低成本等特点，被认为是ORR应用中有前景的材料之一[17]。通过材料系统的巧妙设计，可以制备出三维多孔碳结构，这些结构具有高比表面积和大的孔体积，对于实现高效的ORR至关重要[7,18]。 #### 研究方法与成果本研究提出了一种简单且经济的方法来制备氮掺杂碳网络，用于高效氧还原反应的应用。该方法利用石墨碳氮化物（g-C3N4）作为模板和氮源，同时采用多巴胺作为碳源。通过简单的水热处理和烧结过程，成功合成了具有高比表面积、有效ORR活性和优异稳定性的氮掺杂碳网络结构[1]。具体的合成过程包括：将g-C3N4与多巴胺混合，并进行水热处理；随后，在一定温度下进行烧结，以去除模板并形成所需的多孔结构。这种方法避免了通常涉及多步骤操作、有毒试剂使用以及模板移除过程中可能遇到的复杂问题，从而简化了三维碳结构的制备过程。 #### 材料特性分析 - **比表面积**：合成的氮掺杂碳网络展现出较高的比表面积，这对于提高催化效率至关重要。高比表面积意味着更多的活性位点可用于催化反应，进而提高了整个材料的催化性能。 - **孔隙结构**：通过扫描电子显微镜（SEM）、透射电子显微镜（TEM）等手段，观察到了规则排列的多孔结构，这种结构有利于物质传输和反应过程中的气体扩散。 - **氮掺杂效应**：氮元素的成功掺入进一步增强了材料的电子传输能力和催化活性。氮原子可以通过与碳原子形成特殊键合结构，改变碳网络的电子状态，从而促进氧分子的吸附和转化过程。 #### 应用前景与结论本研究所提出的氮掺杂碳网络不仅具有高效的ORR活性，而且具备出色的稳定性和耐久性，这使得它们在实际应用中具有巨大的潜力。特别是在燃料电池技术领域，这类材料有望替代传统的铂基催化剂，降低生产成本，提高能源转换效率。此外，由于其制备过程简单且环保，也为大规模生产和商业化应用奠定了坚实的基础。该研究成果为开发高效、低成本的ORR催化剂提供了一条新的途径，对推动清洁能源技术的发展具有重要意义。 ### 参考文献 1. Chenxia Li, Xuesong Li, Xiaojuan Sun, et al. Porous Carbon Networks Derived from Graphitic Carbon Nitride for Efficient Oxygen Reduction Reaction [J]. NANOEXPRESS, 2023. 通过上述研究，我们不仅可以深入了解基于石墨碳氮化物的多孔碳网络在高效氧还原反应中的应用，还能认识到这一领域的最新进展和技术挑战。未来的研究将进一步优化材料性能，探索更广泛的潜在应用。

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NAN O E X P R E S S Open Access

Porous Carbon Networks Derived From

Graphitic Carbon Nitride for Efficient

Oxygen Reduction Reaction

Chenxia Li

, Xuesong Li

, Xiaojuan Sun

, Xueyu Zhang

, Lianfeng Duan

, Xijia Yang

, Liying Wang

and Wei Lü

Abstract

Great efforts have been dedicated to finding economic and efficient oxygen reduction reaction (ORR) for fuel cell

technology. Among various catalysts, N-doped carbon-based nanomaterials have attracted much attention due to

low-cost, noble metal free, and good durability. Herein, we developed a facile and economic strategy to prepare

nitrogen-doped carbon networks for efficient ORR application. The g-C

is used as the template and N source,

and dopamine is used as the carbon source. By simple hydrothermal treatment and sintering, N-doped carbon

network structures with high specific surface area, effective ORR activity, and superior durability could be acquired.

The present strategy is free of involving generally multistep, poisonous reagents, and complication of removing

template for fabrication of 3D carbon structures.

Keywords: Mesoporous carbon, Carbon-based materials, Metal free, Oxygen reduction reaction

Background

The oxygen reduction reaction (ORR) is a crucial step for

further development of clean energy conversion strategies

such as fuel cells and metal-air batteries [1–3]. The trad-

itional Pt-based cathode materials for ORR are generally

suffered from high cost, limited stability, and poor toler-

ance to methanol [1, 4–8]. Therefore, to develop a low

cost, highly active, durable material towards ORR has re-

ceived great attention [9, 10]. Numerous efforts have been

dedicated to searching replacement for Pt-based electroca-

talysts, such as transition-metal catalysts [5, 11–13], and

carbon-based nanomaterials [4, 8, 13–16].

Notably, as metal-free electrocatalysts , carbon-based

nanomaterials are promising materials for ORR due to

good durability, noble metal free, and low-cost [17]. By

elegant design of material system, 3D porous carbon

structures could be achieved and provided high specific

area and pore volume, which is extremely important for

efficient ORR [7, 18]. Desirable three-dimensional car-

bon structures generally derived from various templates

including ice, silica, and polystyrene [19]. The fabrication

of 3D carbon structure generally involved multistep, poi-

sonous reagents, and complication of removing template

[6, 20, 21]. Thus, facile preparation strategy is still a

main obstacle. In addition, the introduction of N atoms

in carbon materials significantly enhances electrocata-

lytic activity thus inducing efficient ORR [22, 23]. Great

efforts have reported N-doped carbon materials by intro-

ducing nitrogen-rich source such a s melamine [24, 25],

urea [26], dopamine [27], and pyrr ole followed by sinter-

ing. For ORR applications, a facile way to realize porous

structure and efficient N doping is still highly desi red.

Herein, we developed a strategy to prepare nitrogen-

doped carbon networks for efficient ORR application

using metal-free graphitic carbon nitride (g-C

) and

dopamine (DA) as N source and C source, respectively.

Metal-free g-C

has been intensively investigated due

to its potential application for photocatalysis [9, 28–30]

and ORR [30–33] etc. The N-doped materials could be

achieved using g-C

as the N source due to its high N

content [20, 23, 34 , 35]. The g-C

is a typical two-di-

mensional conjugated polymer material [36, 37]. It has

received extensive attention as an inexpensive, metal-

free, visible light-responsive photocatalyst [38, 39]. The

g-C

has excellent electronic band structure, surface

International License (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and

reproduction in any medium, provided you give appropriate credit to the original author(s) and the source, provide a link to

the Creative Commons license, and indicate if changes were made.

* Correspondence: lixuesong@ccut.edu.cn; lw771119@hotmail.com

Key Laboratory of Advanced Structural Materials, Ministry of Education &

Advanced Institute of Materials Science, Changchu n University of

Technology, Changchun, Changchun 130012, China

Full list of author information is available at the end of the article

Li et al. Nanoscale Research Letters (2019) 14:249

https://doi.org/10.1186/s11671-019-3073-0

functionalization modification, and high physical and

chemical stability and is non-toxic and rich in raw mate-

rials [40–42]. In addition, the nitrogen content is high,

making it one of the known N-rich compounds [43].

The most important thing is that it has a variety of 2D

or 3D structures that can be obtained by controlling the

synthesis conditions [44–46]. Nitrogen-doped carbon

materials generally have a synthesis temperature above

800 °C, which satisfies the requirements for removing

the template [47]. Therefore, it is possible to utilize g-

that only contains carbon and nitrogen elements

to synthesize N-doped carbon materials [ 48 ]. In the

present work, g-C

is used as a template and N source

simultaneously to prepare porous carbon structures with

high specific surface area (954 m

−1

) and 5.71% N con-

tent is achieved, which exhibits comparable ORR activ-

ity, superior durability, and methanol tolerance to Pt/C

reference electrocatalyst.

Methods

Materials

Potassium hydroxide (KOH) and potassium chloride

(KCl) were obtained from Sinopharm Chemical Reagent

Co., Ltd. Potassium hexacyanoferrate (K

[Fe(CN)

]) were

obtained from Tianjin Yongsheng Fine Chemical Co.,

Ltd. Urea were obtained from Beijing Chemical Corp.

All of the above drugs are analytically pure. Naifon® per-

fluorinated solution (5 wt. % in mixture of lower ali-

phatic alcohols and water, contains 45% water) was

purchased from Sigma-Aldrich.

Synthesis of g-C

Template

Typically, 15 g of urea in 100 mL crucible was kept at

550 °C for 4 h. The g-C

was acquired and grounded

to light yellow powder for later use after cooling to room

temperature.

Synthesis of g-C3N4@dopamine Precursors

0.5 g g-C

was dispersed in 20 mL DA solution. The

concentration of DA was 0.3 M. The mixture was ultra-

sonicated for 2 h and transferred into an autoclave

followed by heating at 120 °C for 10 h. The resulted

sample was centrifuged and washed followed by drying

at 80 °C overnight. Three heating temperatures of 120

°C, 140 °C, and160 °C were used for preparing g-C

PDA precursors, and the corresponding samples

were named g-C

/PDA-120, g-C

/PDA-140, and

g-C

/P DA-160, respectively.

Preparation of Nitrogen-Doped 2D Carbon Materials

The precursors of g-C

/PDA-120, g-C

/PDA-140,

and g-C

/PDA-160 were heated to 900 °C for 2 h in ni-

trogen atmosphere. After cooling to room temperature,

nitrogen-doped porous carbon samples named NC-120,

NC-140, and NC-160 (NC-T) were synthesized. However,

the attempt for further decreasing heating temperature to

100 °C induced very poor coating of DA on g-C

,which

resulted in low yield after sintering at 900 °C. Therefore,

three temperatures of 120 °C, 140 °C, and 160 °C were

chosen for further investigation. The synthesis process of

nitrogen-doped porous carbon samples is shown in

Scheme 1.

Electrochemical Measurement

Electrochemical analysis was fulfilled by the DyneChe m

electrochemical workstation, and Ag/AgCl and platinum

are used as reference electrode and counter electrode,

respectively. The cyclic voltampis wa s tested in 0.1 M

potassium hydroxide solution. The glass carbon elec-

trode (GCE) was polished and washed before usin g. To

prepare the working electrodes, aliquots of 5 μL and 2.5

mg/mL NC-120, NC-140, NC-160, Pt/C solutions were

dipped on to GCE for further test.

Characterization

The structure and chemical composition of the NC-T

was analyzed by X-ray diffraction (XRD) (D-MAX II A

X-ray diffractometer), transmission electron microscopy

(TEM) (Tecnai F20), scanning electron microscope

(SEM) (JEOL7610), fourier transform infrared (FT-IR)

(Nicolet iS50) spectra, X-ray photoelectron spectroscopy

(XPS) (Kratos Axis Ult raDLD), and Raman (Horiba,

Japan); N2 adsorption-desorption (77 K) isotherms were

carried out on a Micromeritics ASAP 2020 instrument

(MICROSENSOR, USA).

Results and Discussion

SEM and TEM Characterization

In order to determine the morphology of the synthesized

samples, SEM and TEM are used for structure observa-

tion as shown in Fig. 1. Figure 1a represents the sheet

structure of as-synthesized g-C

. The 2D structure of

g-C

is further confirmed from Fig. 1b, which is simi-

lar with the previous report [48]. For g-C

/PDA-120

as shown in Fig. 1c, d, the SEM image is similar with

that of g-C

. However, the TEM image of g-C

PDA-120 shows well-dispersed sheet like morphology,

compared with as-synthesized g-C

. With the increas-

ing heating temperature from 120 to 160 °C, the thin la-

mellar structure of carbonized layer could be observed

(Additional file 1: Figure S1). After sintering at 900 °C,

the SEM images appear honeycomb-like structures as

shown in Fig. 1e due to the pyrolysis of g-C

template,

inducing porous carbon structures as shown in Fig. 1fand

Additional file 1: Figure S2. The thermo-gravity test of g-

was carried out to determine the residue of g-C

and g-C

begins to decompose at 520 °C. Under nitro-

gen protection, fully decomposition is confirmed at 760 °C

Li et al. Nanoscale Research Letters (2019) 14:249 Page 2 of 9

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