Hypercrosslinked polymers enabled micropore-dominant N, S Co-Doped porous carbon for ultrafast electron/ion transport supercapacitors

Lu, Yun; Liang, Jianing; Deng, Shaofeng; He, Qiming; Deng, Shuyi; Hu, Yezhou; Wang, Deli

doi:10.1016/j.nanoen.2019.103993

Cited by 207 publications

(98 citation statements)

References 50 publications

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“…The σ value is impressively small given that the majority of charge is stored through pseudocapacitive reactions. It is even smaller than the values reported for carbon fibers (3.33 Ω s −0.5 ), mesoporous carbon fibers (0.64 Ω s −0.5 ), and most other carbon‐based materials . Taken together, these results unambiguously confirmed the critical role of 3D‐printed periodic porous structure in facilitating ion diffusion and accessibility.…”

Section: Methodssupporting

confidence: 56%

“…It is even smaller than the values reported for carbon fibers (3.33 Ω s −0.5 ), mesoporous carbon fibers (0.64 Ω s −0.5 ), and most other carbon-based materials. [64,71,73] Taken together, these results unambiguously confirmed the critical role of 3D-printed periodic porous structure in facilitating ion diffusion and accessibility. The fast kinetics of SF-3D GA makes it a unique and attractive pseudocapacitive electrode for fast-charging devices.…”

supporting

confidence: 63%

“…The capacitance contribution from the fast kinetic process (yellow region) is dominant at all potentials, with a total contribution of 93.3%. This value is much higher than the values reported for other pseudocapacitive materials at the same scan rate, demonstrating the excellent ion accessibility of the SF‐3D GA electrode . In contrast, the SF‐GA only has 75.8% of the capacitance that comes from the fast kinetic process.…”

Section: Methodsmentioning

confidence: 57%

“…This value is much higher than the values reported for other pseudocapacitive materials at the same scan rate, demonstrating the excellent ion accessibility of the SF-3D GA electrode. [64,[69][70][71] In contrast, the SF-GA only has 75.8% of the capacitance that comes from the fast kinetic process. Furthermore, we compared the ion diffusion resistances (σ) of SF-3D GA and SF-GA obtained in the same electrolyte and at the same potential; the values of σ should be related to the electrode structure and charge storage mechanism.…”

mentioning

confidence: 99%

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3D‐Printed Structure Boosts the Kinetics and Intrinsic Capacitance of Pseudocapacitive Graphene Aerogels

et al. 2020

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The performance of pseudocapacitive electrodes at fast charging rates are typically limited by the slow kinetics of Faradaic reactions and sluggish ion diffusion in the bulk structure. This is particularly problematic for thick electrodes and electrodes highly loaded with active materials. Here, a surface‐functionalized 3D‐printed graphene aerogel (SF‐3D GA) is presented that achieves not only a benchmark areal capacitance of 2195 mF cm−2 at a high current density of 100 mA cm−2 but also an ultrahigh intrinsic capacitance of 309.1 µF cm−2 even at a high mass loading of 12.8 mg cm−2. Importantly, the kinetic analysis reveals that the capacitance of SF‐3D GA electrode is primarily (93.3%) contributed from fast kinetic processes. This is because the 3D‐printed electrode has an open structure that ensures excellent coverage of functional groups on carbon surface and facilitates the ion accessibility of these surface functional groups even at high current densities and large mass loading/electrode thickness. An asymmetric device assembled with SF‐3D GA as anode and 3D‐printed GA decorated with MnO2 as cathode achieves a remarkable energy density of 0.65 mWh cm−2 at an ultrahigh power density of 164.5 mW cm−2, outperforming carbon‐based supercapacitors operated at the same power density.

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Section: Methodssupporting

confidence: 56%

supporting

confidence: 63%

Section: Methodsmentioning

confidence: 57%

mentioning

confidence: 99%

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3D‐Printed Structure Boosts the Kinetics and Intrinsic Capacitance of Pseudocapacitive Graphene Aerogels

et al. 2020

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“…Concretely, thiophene/pyrrole (Th/Py) monomers were initiated by the cationic catalyst (FeCl 3 ) and formed numerous 1D polymer flexible segments. Subsequently, each segments are closely linked with neighbors and further forming 2D networks or even 3D rigid crosslinking agents, which are so called hypercrosslinked polymers (HCPs) . Such one step cationic hypercrosslinked strategy has achieved an ideal phase transformation processes from initial 0D micromolecule monomer to final 3D HCPs.…”

Section: Resultsmentioning

confidence: 99%

Accurate Control Multiple Active Sites of Carbonaceous Anode for High Performance Sodium Storage: Insights into Capacitive Contribution Mechanism

Liang

et al. 2020

Advanced Energy Materials

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Heteroatom doping is widely recognized as an appealing strategy to break the capacitance limitation of carbonaceous materials toward sodium storage. However, the concrete effects, especially for heteroatomic phase transformation, during the sodium storage reaction remain a confusing topic. Here, a novel hypercrosslinked polymerization approach is demonstrated to fabricate pyrrole/thiophene hypercrosslinked microporous copolymer and further give porous carbonaceous materials with accurately regulated N/S dual doping corresponding to starting feeding ratios. Significantly, the N doping contributes to the conductivity and surface wettability, while the S doping is bridged to build stable active sites, which can be electrochemically converted into mercaptan anions via faraday reaction and further enhancing reversible capacities. Meanwhile, the abundant S doping can also conduce to the expanded interlayer spacing to shorten the ions diffusion distance, thus optimizing the reaction kinetic. As a result, the N0.2S0.8‐micro‐dominant porous carbon delivers the highest reversible capacity of 521 mAh g−1 at 100 mA g−1 and excellent cyclic stability over 2000 cycles at 2000 mA g−1 with a capacity decay of 0.0145 mAh g−1 per cycle. This work is anticipated to provide an in‐depth understanding of capacitance contribution and illuminate the heteroatomic phase transformation during sodium storage reactions for doping carbonaceous anodes.

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Multiple Active Sites Carbonaceous Anodes for Na⁺ Storage: Synthesis, Electrochemical Properties and Reaction Mechanism Analysis

Shin

et al. 2020

Adv Funct Materials

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Owing to the earth‐abundant resources, cost effective materials and stable electrochemical properties, sodium‐ions batteries (SIBs) show long‐term potential in responding to the rapid consumption of lithium resources and the ever‐increasing development of new energy storage devices. Nevertheless, the intrinsic properties of the large ion radius (Na+ 1.02 Å vs Li+ 0.76 Å) and positive reduction potential (Na/Na+ −2.71 V vs Li/Li+ −3.04 V) may impede ion diffusion, thus causing serious volume expansion, resulting in poor cycling stability. To address these issues, the incorporation of active sites into carbonaceous anode is considered as an efficient strategy to enhance interfacial compatibility, enlarge interlayer distance, and supply reversible Faradic pseudo‐capacitance. Herein, the multiple active sites carbonaceous anodes for SIBs anode are comprehensively reviewed. Typically, carbonaceous materials are categorized into diffusion and surface controlled based on Na storage mechanism, and the concepts of intrinsic/extrinsic active sites are proposed according to the types of active sites. Furthermore, to reveal the reaction kinetics and guide the rational design of high performance anodes, the (spectro) electrochemical analysis methods and corresponding key parameters are introduced. Additionally, primary superiorities, essential issues, and supposed solutions of multiple active sites carbonaceous Na anodes are discussed and the future development directions are also proposed. This review may provide new design thoughts for high performance carbonaceous Na storage anodes.

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Hypercrosslinked polymers enabled micropore-dominant N, S Co-Doped porous carbon for ultrafast electron/ion transport supercapacitors

Cited by 207 publications

References 50 publications

3D‐Printed Structure Boosts the Kinetics and Intrinsic Capacitance of Pseudocapacitive Graphene Aerogels

3D‐Printed Structure Boosts the Kinetics and Intrinsic Capacitance of Pseudocapacitive Graphene Aerogels

Accurate Control Multiple Active Sites of Carbonaceous Anode for High Performance Sodium Storage: Insights into Capacitive Contribution Mechanism

Multiple Active Sites Carbonaceous Anodes for Na⁺ Storage: Synthesis, Electrochemical Properties and Reaction Mechanism Analysis

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Hypercrosslinked polymers enabled micropore-dominant N, S Co-Doped porous carbon for ultrafast electron/ion transport supercapacitors

Cited by 207 publications

References 50 publications

3D‐Printed Structure Boosts the Kinetics and Intrinsic Capacitance of Pseudocapacitive Graphene Aerogels

3D‐Printed Structure Boosts the Kinetics and Intrinsic Capacitance of Pseudocapacitive Graphene Aerogels

Accurate Control Multiple Active Sites of Carbonaceous Anode for High Performance Sodium Storage: Insights into Capacitive Contribution Mechanism

Multiple Active Sites Carbonaceous Anodes for Na+ Storage: Synthesis, Electrochemical Properties and Reaction Mechanism Analysis

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Multiple Active Sites Carbonaceous Anodes for Na⁺ Storage: Synthesis, Electrochemical Properties and Reaction Mechanism Analysis