Carbon‐Based Metal‐Free Catalysts for Energy Storage and Environmental Remediation

Hu, Chuangang; Lin, Yi; Connell, John W.; Cheng, Hui‐Ming; Gogotsi, Yury; Titirici, Maria‐Magdalena; Dai, Liming

doi:10.1002/adma.201806128

Cited by 222 publications

(104 citation statements)

References 156 publications

(196 reference statements)

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“…The overuse of fossil fuel has caused a rapid increase in CO 2 emissions and the associated severe environmental issues, including global warming, polar ice melting, sea level rising, rain acidification, and species extinction. [ 1,2 ] As a new strategy for CO 2 sequestration and environmental remediation, the utilization of CO 2 in metal (Li)–CO 2 batteries with a high theoretical specific capacity has recently attracted considerable attention. [ 3,4 ] Apart from the CO 2 sequestration, Li–CO 2 batteries offer an advantage for energy conversion and storage, particularly for exploration of the planet Mars with an atmosphere consisting of 96% CO 2 .…”

Section: Methodsmentioning

confidence: 99%

“…[ 5–7,9,10 ] Apart from their high cost, however, the use of a high content of heavy metals (ions) could not only decrease the gravimetric energy density of a battery, but also cause detrimental effects on the environmental safety and electrolyte stability. [ 11 ] Therefore, considerable effort has been devoted to the design and development of carbon‐based metal‐free electrocatalysts (C‐MFECs) as air cathodes in Li–CO 2 batteries, [ 2,12–14 ] though their efficiency and/or stability need to be further improved. On the other hand, single‐atom catalysts (SACs) have recently attracted a great deal of interest for various reactions, [ 15–19 ] including CO 2 reduction and evolution in batteries.…”

Section: Methodsmentioning

confidence: 99%

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High‐Performance, Long‐Life, Rechargeable Li–CO₂ Batteries based on a 3D Holey Graphene Cathode Implanted with Single Iron Atoms

et al. 2020

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for CO 2 sequestration and environmental remediation, the utilization of CO 2 in metal (Li)-CO 2 batteries with a high theoretical specific capacity has recently attracted considerable attention. [3,4] Apart from the CO 2 sequestration, Li-CO 2 batteries offer an advantage for energy conversion and storage, particularly for exploration of the planet Mars with an atmosphere consisting of 96% CO 2 . [3] The driving force for energy conversion and storage in Li-CO 2 batteries is the reversible redox reaction between a lithium anode and CO 2 gas cathode to form/decompose Li 2 CO 3 during the discharge/charge processes. The sluggish CO 2 reduction and evolution reactions that take place at the air cathode often impede the kinetics of Li-CO 2 batteries, leading to a high voltage (>4.5 V vs Li/Li + ) for decomposing the discharge product (Li 2 CO 3 ). [5][6][7] Under such a high anodic potential, the electrolyte oxidation limits the energy efficiency and cycling life of the Li-CO 2 batteries. [5][6][7] Therefore, efficient A highly efficient cathode catalyst for rechargeable Li-CO 2 batteries is successfully synthesized by implanting single iron atoms into 3D porous carbon architectures, consisting of interconnected N,S-codoped holey graphene (HG) sheets. The unique porous 3D hierarchical architecture of the catalyst with a large surface area and sufficient space within the interconnected HG framework can not only facilitate electron transport and CO 2 /Li + diffusion, but also allow for a high uptake of Li 2 CO 3 to ensure a high capacity. Consequently, the resultant rechargeable Li-CO 2 batteries exhibit a low potential gap of ≈1.17 V at 100 mA g −1 and can be repeatedly charged and discharged for over 200 cycles with a cut-off capacity of 1000 mAh g −1 at a high current density of 1 A g −1 . Density functional theory calculations are performed and the observed appealing catalytic performance is correlated with the hierarchical structure of the carbon catalyst. This work provides an effective approach to the development of highly efficient cathode catalysts for metal-CO 2 batteries and beyond.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adma.201907436.The overuse of fossil fuel has caused a rapid increase in CO 2 emissions and the associated severe environmental issues, including global warming, polar ice melting, sea level rising, rain acidification, and species extinction. [1,2] As a new strategy

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Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

High‐Performance, Long‐Life, Rechargeable Li–CO₂ Batteries based on a 3D Holey Graphene Cathode Implanted with Single Iron Atoms

et al. 2020

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“…Highly redox active materials are an important tool for the degradation of refractory organic water and soil contaminants. [ 1–7 ] Nanoscale zero valent (NZVI) has been used for in situ groundwater remediation for more than two decades. [ 8–12 ] NZVI is a strong reductant that readily dechlorinates chlorinated solvents and antibiotics, and reduces and immobilizes heavy metals and radionuclides.…”

Section: Figurementioning

confidence: 99%

Sulfur Loading and Speciation Control the Hydrophobicity, Electron Transfer, Reactivity, and Selectivity of Sulfidized Nanoscale Zerovalent Iron

et al. 2020

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radionuclides. [12][13][14][15][16][17] However, NZVI is an indiscriminate reductant that also readily reduces water to form hydrogen gas (Fe 0 + 2H 2 O → Fe 2+ + 2OH − + H 2(g) ). [18] This unwanted side reaction consumes the reducing capacity of the NZVI, decreasing its reactive lifetime, and increases the amount and cost of NZVI required for remediation. Several approaches have been proposed to increase the reactivity or stability of NZVI during remediation, including encapsulating them with polymers or into silica matrices, [15,19] doping them with noble metals like Pd or Pt, [20,21] and supporting them onto carbon matrices like carbon nanotubes or graphene. [22,23] While these approaches improve the injectability of the materials into the subsurface, none have improved the selectivity of NZVI for contaminants over water while still maintaining high reactivity with the target groundwater contaminants. An ideal material for groundwater remediation should possess both high reactivity and selectivity, [24] where the contaminant outcompetes water for reactive sites.Recently, it was shown by us and others that the sulfidation of NZVI lowers its reactivity with water and other non-target hydrophilic contaminants (e.g., NO 3 − ), while increasing its reactivity with target contaminants like chlorinated solvents Sulfidized nanoscale zerovalent iron (SNZVI) is a promising material for groundwater remediation. However, the relationships between sulfur content and speciation and the properties of SNZVI materials are unknown, preventing rational design. Here, the effects of sulfur on the crystalline structure, hydrophobicity, sulfur speciation, corrosion potential, and electron transfer resistance are determined. Sulfur incorporation extended the nano-Fe 0 BCC lattice parameter, reduced the Fe local vacancies, and lowered the resistance to electron transfer. Impacts of the main sulfur species (FeS and FeS 2 ) on hydrophobicity (water contact angles) are consistent with density functional theory calculations for these FeS x phases. These properties well explain the reactivity and selectivity of SNZVI during the reductive dechlorination of trichloroethylene (TCE), a hydrophobic groundwater contaminant. Controlling the amount and speciation of sulfur in the SNZVI made it highly reactive (up to 0.41 L m −2 d −1 ) and selective for TCE degradation over water (up to 240 moles TCE per mole H 2 O), with an electron efficiency of up to 70%, and these values are 54-fold, 98-fold, and 160-fold higher than for NZVI, respectively. These findings can guide the rational design of robust SNZVI with properties tailored for specific application scenarios.Highly redox active materials are an important tool for the degradation of refractory organic water and soil contaminants. [1][2][3][4][5][6][7] Nanoscale zero valent (NZVI) has been used for in situ groundwater remediation for more than two decades. [8][9][10][11][12] NZVI is a strong reductant that readily dechlorinates chlorinated solvents and antibiotics, and reduces and immobilizes h...

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“…Efficient and inexpensive energy storage devices are urgently needed to support widespread application of renewable energy and smart grid development . Recently, as a new type of energy storage device between traditional capacitor and battery, supercapacitor has been applied in various fields due to its high power density, long cycle life, and friendly environment .…”

Section: Introductionmentioning

confidence: 99%

Aniline‐grafting graphene oxide/polyaniline composite prepared via interfacial polymerization with high capacitive performance

Wang

et al. 2019

Int J Energy Res

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Summary Polyaniline (PANI), a low‐cost conducting polymer with an excellent specific capacitance and a high conductivity, is a promising organic material served for supercapacitor. However, it tends to curl and swell after constant charge and discharge, resulting in poor cycle stability. In this work, we employed the interfacial polymerization route to construct an aniline‐grafting graphene oxide/PANI (GO‐ANI/PANI) composite. The as‐prepared GO‐ANI/PANI composite shows a high specific capacitance (160.5 F g‐1) at 0.5 A g‐1 under the wide potential range from 0.0 to 1.0 V. Importantly, at a high current density (10 A g‐1), the capacitance retains 86% after 3000 cycles due to the enhanced interaction between GO and PANI and good conductive network. It has been demonstrated that the GO‐ANI/PANI composite has a higher specific capacitance and better stability compared with GO/PANI obtained by common method. This study implies that the composite electrode could be a competitive candidate for high‐performance supercapacitor.

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Carbon‐Based Metal‐Free Catalysts for Energy Storage and Environmental Remediation

Cited by 222 publications

References 156 publications

High‐Performance, Long‐Life, Rechargeable Li–CO₂ Batteries based on a 3D Holey Graphene Cathode Implanted with Single Iron Atoms

High‐Performance, Long‐Life, Rechargeable Li–CO₂ Batteries based on a 3D Holey Graphene Cathode Implanted with Single Iron Atoms

Sulfur Loading and Speciation Control the Hydrophobicity, Electron Transfer, Reactivity, and Selectivity of Sulfidized Nanoscale Zerovalent Iron

Aniline‐grafting graphene oxide/polyaniline composite prepared via interfacial polymerization with high capacitive performance

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Carbon‐Based Metal‐Free Catalysts for Energy Storage and Environmental Remediation

Cited by 222 publications

References 156 publications

High‐Performance, Long‐Life, Rechargeable Li–CO2 Batteries based on a 3D Holey Graphene Cathode Implanted with Single Iron Atoms

High‐Performance, Long‐Life, Rechargeable Li–CO2 Batteries based on a 3D Holey Graphene Cathode Implanted with Single Iron Atoms

Sulfur Loading and Speciation Control the Hydrophobicity, Electron Transfer, Reactivity, and Selectivity of Sulfidized Nanoscale Zerovalent Iron

Aniline‐grafting graphene oxide/polyaniline composite prepared via interfacial polymerization with high capacitive performance

Contact Info

Product

Resources

About

High‐Performance, Long‐Life, Rechargeable Li–CO₂ Batteries based on a 3D Holey Graphene Cathode Implanted with Single Iron Atoms

High‐Performance, Long‐Life, Rechargeable Li–CO₂ Batteries based on a 3D Holey Graphene Cathode Implanted with Single Iron Atoms