Hierarchical N-doped porous carbon hosts for stabilizing tellurium in promoting Al-Te batteries

doi:10.1016/j.jechem.2020.09.015

Journal of Energy Chemistry

Volume 57, June 2021, Pages 378-385

https://doi.org/10.1016/j.jechem.2020.09.015 Get rights and content

Highlights

•
A nitrogen doped porous (N-PC) carbon is derived from zeolite imidazolate framework.
•
The reduced graphene oxide (rGO) nanosheets are introduced to form a stable host for stabilizing Te.
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N-PC exhibits significantly efficient to improving the chemical and electrochemical dissolution of Te.

Abstract

Aluminum batteries are attractive in electrochemical energy storage due to high energy density and low-cost aluminum, while the energy density is limited for the lack of favorable positive electrode materials to match aluminum negative electrodes. Tellurium positive electrode is intrinsically electrically conductive among chalcogen and holds high theoretical specific capacity (1260.27 mAh g⁻¹) and discharge voltage plateau (~1.5 V). However, the chemical and electrochemical dissolution of Te active materials results in the low material utilization and poor cycling stability. To enhance the electrochemical performance, herein a nitrogen doped porous carbon (N-PC) is derived from zeolite imidazolate framework (ZIF-67) as an effective tellurium host to suppress the undesired shuttle effect. In order to inhibit the volume expansion of N-PC during the charge/discharge process, the reduced graphene oxide (rGO) nanosheets are introduced to form a stable host materials (N-PC-rGO) for stabilizing Te. The physical encapsulation and chemical confinement to soluble tellurium species are achieved. N-PC-rGO-Te positive electrode exhibits an improved initial specific capacity and long-term cycling performance at a current density of 500 mA g⁻¹ (initial specific capacity: 935.5 mAh g⁻¹; after 150 cycles: 467.5 mAh g⁻¹), highlighting a promising design strategy for inhibiting chemical and electrochemical dissolution of Te.

Graphical abstract

Hierarchical N-doped porous carbon is used as the host of tellurium to fabricate the high-capacity and stable Al-Te batteries, highlighting a promising approach for assembling high-performance aluminum ions batteries.

Introduction

The ever-growing demand for portable electronics, smart grids, and electric vehicles has stimulated extensive researches on energy conversion and storage devices with high energy densities. Especially, aluminum ion batteries (AIBs) have drawn significant attention for their favorable energy-to-price ratios and high energy density of aluminum and safe feature. So far, numerous researches have been involved to develop positive electrode materials, including graphitic materials [1], [2], [3], [4], metal oxides [5], [6], [7], [8], sulfides [9], [10], selenides [11], [12], elemental sulfur [13], [14], [15], [16], and selenium [17], while they are still insufficient to deliver desirable energy density. As a positive electrode material, Sulfur has been regarded as one of the most promising candidates for advanced energy storage materials due to its high theoretical specific energy of 2600 Wh kg⁻¹ as well as natural abundance and environmental benignity. However, the critical problems, including poor electronic conductivity (5 × 10⁻¹⁶ S m⁻¹) [18] of sulfur, large volume expansion during the charge/discharge process and shuttle effect of polysulfide, have seriously hindered the development of Al-S batteries.

From the same family of chalcogen, tellurium is known to have higher electronic conductivity (2 × 10⁻⁴ S m⁻¹) [19] than sulfur and selenium (1 × 10⁻¹⁰ S m⁻¹) [18] and holds high theoretical specific capacity (~1260.27 mA h g⁻¹ and discharge voltage plateau at ~1.5 V). Notably, the theoretical capacity of Al-Te battery system is higher than that of Li-Te battery system (420 mA h g⁻¹), which is attributed to multi-step redox process of Te (i.e., six electronics were transferred during the oxidation or reduction process). However, the chemical dissolution (tellurium spontaneously reacts chemically in Lewis acidic electrolyte) and electrochemical dissolution in the electrolyte leads to low active material utilization and poor initial discharge capacity in our previous work [20]. Although the porous carbon-based modified separator was able to enhance electrochemical performance of Al-Te battery, the actual energy density of the battery was also attenuated due to the high mass density of SWCNT and low active material loading (43.5%). Therefore, one promising strategy is to develop rational positive electrodes, with purpose of enhancing the utilization of active materials while blocking the shuttle effects in Al-Te batteries (ATBs).

To effectively utilize Te active materials at positive electrodes, here reduced graphene oxide (rGO) wrapped MOFs-derived nitrogen doped porous carbon (N-PC) was designed as the host of tellurium. In such design, the C-Co-N in N-PC can immobilize the soluble tellurium compounds via chemical interaction, and meanwhile the tightly wrapped rGO nanosheets could act as the barrier layers to prevent soluble tellurium compounds as a result of suppressing shuttle effect (Fig. S1). As expected, much promoted initial specific capacity (935.5 mA h g⁻¹) could be achieved, along with much prolonged stable cycling performance obtained. The results and analysis imply the efficiency design for improving the electrochemical process in the ATBs using such hierarchical nanostructure.

Section snippets

Synthesis of ZIF-67 and N-PC

All chemicals and solvents were purchased from commercial sources and used without further purification. In a typical synthesis process, 5.238 g Co(NO₃)₂∙6H₂O and 3.955 g 2-methylimidazole were dissolved in 200 mL of methanol, respectively. Then the 2-methylimidazole solution was slowly poured into the solution of Co(NO₃)₂∙6H₂O under string and the mixed two solutions were kept at the room temperature for 20 h. The final precipitates (ZIF-67) were collected by centrifugation, washed with

Results and discussion

In the design of ATBs, two types of positive electrodes, i.e. nitrogen doped porous carbon loaded tellurium (N-PC-Te) and reduced graphene oxide wrapped nitrogen doped porous carbon loaded tellurium (N-PC-rGO-Te), were directly employed as the active material in the positive electrode without further modification. By mixing the active materials with amorphous carbon and binders, the as-prepared mixtures were used as the positive electrode (Fig. 1(a and b)). According to our recent study [20],

Conclusions

N-PC and N-PC-rGO host materials to tellurium positive electrode for aluminum batteries were rationally designed and prepared. The results reveal that N-PC can improve the chemical and electrochemical dissolution of Te. However, N-PC-Te nanostructure is still easily destroyed at high current densities, resulting in rapid decline of capacity and poor cycling stability. Consequently, the reduced graphene oxide is introduced to stabilize the structure of N-PC and thereby achieving high capacity

Declaration of Competing Interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgments

This work was supported by the National Natural Science Foundation of China (No. 51725401 and 51874019) and the Fundamental Research Funds for the Central Universities (FRF-TP-17-002C2).

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Due to the high microporous structure and controllable morphology, zeolitic imidazolate framework is a typical representative of metal organic frameworks (MOFs) that manufactured by a facile method at low cost and can be served as an attractive precursor with excellent electrochemical activity to fabricate 3D structured nanocarbon, metal oxides and nitrides [19–22]. As the carbon-based Co3O4 hybrids derived from the calcination of ZIF-67 in air possess the advantageous 3D structure and abundant active sites [23]. There upon, to fabricate MOF-derived Co3O4 hybrids will be propitious to the attachment and permeation of the oxygen and electrolyte, which hopefully leads to achieve a satisfactory catalytic performance towards H2O2 electroreduction.
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View full text

Hierarchical N-doped porous carbon hosts for stabilizing tellurium in promoting Al-Te batteries

Highlights

Abstract

Graphical abstract

Introduction

Section snippets

Synthesis of ZIF-67 and N-PC

Results and discussion

Conclusions

Declaration of Competing Interest

Acknowledgments

Energy Storage Mater.

J. Power Sources

J. Power Sources

Chem

Mater. Today Energy

Biosens. Bioelectron.

Electrochim. Acta

J. Electrochem. Soc.

Adv. Mater.

Adv. Energy Mater.

J. Mater. Chem. A

ACS Sustain. Chem. Eng.

ACS Appl. Nano Mater.

Adv. Energy Mater.

Adv. Mater.

ACS Appl. Mater. Interfaces

Sustainable Energy Fuels

Electron. Mater. Lett.