Metal-free carbon-based catalysts design for oxygen reduction reaction towards hydrogen peroxide: From 3D to 0D

Zhang, Ding; Mitchell, Ellen M.; Lu, Xunyu; Chu, Dewei; Shang, Lu; Zhang, Tierui; Amal, Rose; Han, Zhaojun

doi:10.1016/j.mattod.2023.02.004

Cited by 35 publications

(22 citation statements)

References 123 publications

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“…The above results prove that the incorporation of carbon matrix is essential to enhance the HER activity of NiSe 2 . In addition, the hierarchical pores involved in NC provide rich channels for the efficient transport of active species in the catalytic process of electrocatalysis, thereby significantly boosting the electrochemical performance …”

Section: Resultsmentioning

confidence: 66%

“…45 In addition, the hierarchical pores involved in NC provide rich channels for the efficient transport of active species in the catalytic process of electrocatalysis, thereby significantly boosting the electrochemical performance. 46 To understand the intrinsic mechanism of high catalytic activity of NC-NiSe 2 -x, the HER kinetics are further studied by Tafel slopes, where a smaller value is indicative of faster reaction kinetics. 47 As observed in Figure 5b 49 The turnover frequency (TOF) values of NC-NiSe 2 -x are calculated (Figure S7), and the number of active sites is estimated based on the active Ni sites determined from the redox reaction of Ni species at different CV scan rates.…”

Section: Structural and Morphological Analysesmentioning

confidence: 99%

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Coupling NiSe₂ Nanoparticles with N-Doped Porous Carbon Enables Efficient and Durable Electrocatalytic Hydrogen Evolution Reaction at pH Values Ranging from 0 to 14

He,

Chen,

Meng

et al. 2023

ACS Appl. Nano Mater.

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Integrating metal-based species with a carbon matrix is a promising approach for fabricating inexpensive, durable, and efficient electrocatalysts. Herein, NiSe 2 -decorated and N-doped carbon polyhedra (NC) are prepared as electrocatalysts for hydrogen evolution reaction (HER) by a template-assisted approach. The optimal NC-NiSe 2 delivers extraordinary catalytic activities toward HER in a wide pH range, with overpotentials of 127 mV in 0.5 M H 2 SO 4 , 226 mV in 1 M PBS, and 205 mV in 1 M KOH to drive a current density of 10 mA cm −2 . In addition, this catalyst undergoes fast reaction kinetics via a Volmer−Heyrovsky mechanism and exhibits excelent long-term catalytic durability for 48 h in the full pH media. During electrocatalysis, when electrons pass through the NC matrix to the surface of NiSe 2 particles, water molecules at the active sites of NiSe2 are reduced, and then hydrogen is released. The excellent catalytic activity and durability mainly benefit from the hierarchically porous architecture as well as the synergistic interaction of NiSe 2 nanoparticles and NC matrix, which not only significantly boost the electronic conductivity and generate plentiful active sites but also guarantee the chemical and structural stabilities of NiSe 2 catalytic species. This work unravels deep insights into the exploration of carbonsupported metal chalcogenides as highly efficient HER electrocatalysts at full-pH values.

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Section: Resultsmentioning

confidence: 66%

Section: Structural and Morphological Analysesmentioning

confidence: 99%

Coupling NiSe₂ Nanoparticles with N-Doped Porous Carbon Enables Efficient and Durable Electrocatalytic Hydrogen Evolution Reaction at pH Values Ranging from 0 to 14

He,

Chen,

Meng

et al. 2023

ACS Appl. Nano Mater.

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“…This can be stopped with a new class of materials in which there is complete absence of metals. Development of metal free materials is not new, and it is preceded by a class of metal free homogeneous catalysts known as “organo-catalysts”. One of the earliest organocatalyzed reactions known is the utilization of cinchona alkaloids for the addition of hydrogen cyanide (HCN) to aldehydes, which was first published in 1912 by Bredig and Fiske .…”

Section: Introductionmentioning

confidence: 99%

Metal-Free Carbon-Based Nanomaterials: Insights from Synthesis to Applications in Sustainable Catalysis

Jaryal,

Villa,

Gupta

2023

ACS Sustainable Chem. Eng.

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The development of cutting-edge catalysts is critical in material science for sustainable development. Though, metals have always been used in catalysis for enabling essential chemicals, but their use is not considered sustainable owing to the high cost, toxicity, and poor durability. Nevertheless, the modern focus has shifted towards metal free materials due to their leading role in sustainable development. Carbon-based nanomaterials have become focus of researchers over last 30 years and are used either as a catalyst support or metal-free catalyst in various chemical conversions. They are highly anticipated as state-of-the-art materials due to high specific surface area, high conductivity, and tunable functional groups. This account summarizes various strategies proposed by our group to design metal-free carbon catalysts for electrochemical sensing, biomass valorization, and synthesis of value-added chemicals. Also, "metal-free" point-of-care devices are fabricated to provide affordable healthcare services to the user end. The materials are designed using graphitic carbon nitride, reduced graphene oxide, Janus 2D carbon nanomaterials, ultradispersed diamonds, and carbon nanotubes. Their efficacy can be improved by building composites with metal-free materials and incorporating defects. Finally, we share some knowledge and insights regarding current challenges and future perspectives in this emerging field.

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“…[16] For practical implementation, metal-free photocatalysts would be much more favorable, particularly carbonaceous materials, as they are naturally abundant, inexpensive, environmentally friendly, and chemically and mechanically stable. [17] Carbon nitride polymers and reduced graphene oxide are utilized in various photocatalytic applications. [18][19][20][21][22][23][24][25] Their optoelectronic properties can be influenced by "proper" synthesis.…”

Section: Introductionmentioning

confidence: 99%

Bandgap Engineering of Melon using Highly Reduced Graphene Oxide for Enhanced Photoelectrochemical Hydrogen Evolution

et al. 2023

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The uncondensed form of polymeric carbon nitrides (PCN), generally known as melon, is a stacked two‐dimensional structure of poly(aminoimino)heptazine. Melon is used as a photocatalyst in solar energy conversion applications, but suffers from a poor photoconversion efficiency due to weak optical absorption in the visible spectrum, high activation energy, and inefficient separation of photoexcited charge carriers. We report experimental and theoretical studies to engineer the bandgap of melon with highly reduced graphene oxide (HRG). Three HRG@melon nanocomposites with different HRG:melon ratios (0.5%, 1%, and 2%) were prepared. The 1% HRG@melon nanocomposite showed a higher photocurrent density (71 μA cm−2) than melon (24 μA cm−2) in alkaline conditions. The addition of a hole scavenger further increased the photocurrent density to 630 μA cm−2 relative to the reversible hydrogen electrode (RHE). These experimental results were validated by calculations using density functional theory (DFT), which revealed that HRG results in a significant charge redistribution and an improved photocatalytic hydrogen evolution reaction (HER).This article is protected by copyright. All rights reserved

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Metal-free carbon-based catalysts design for oxygen reduction reaction towards hydrogen peroxide: From 3D to 0D

Cited by 35 publications

References 123 publications

Coupling NiSe₂ Nanoparticles with N-Doped Porous Carbon Enables Efficient and Durable Electrocatalytic Hydrogen Evolution Reaction at pH Values Ranging from 0 to 14

Coupling NiSe₂ Nanoparticles with N-Doped Porous Carbon Enables Efficient and Durable Electrocatalytic Hydrogen Evolution Reaction at pH Values Ranging from 0 to 14

Metal-Free Carbon-Based Nanomaterials: Insights from Synthesis to Applications in Sustainable Catalysis

Bandgap Engineering of Melon using Highly Reduced Graphene Oxide for Enhanced Photoelectrochemical Hydrogen Evolution

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Metal-free carbon-based catalysts design for oxygen reduction reaction towards hydrogen peroxide: From 3D to 0D

Cited by 35 publications

References 123 publications

Coupling NiSe2 Nanoparticles with N-Doped Porous Carbon Enables Efficient and Durable Electrocatalytic Hydrogen Evolution Reaction at pH Values Ranging from 0 to 14

Coupling NiSe2 Nanoparticles with N-Doped Porous Carbon Enables Efficient and Durable Electrocatalytic Hydrogen Evolution Reaction at pH Values Ranging from 0 to 14

Metal-Free Carbon-Based Nanomaterials: Insights from Synthesis to Applications in Sustainable Catalysis

Bandgap Engineering of Melon using Highly Reduced Graphene Oxide for Enhanced Photoelectrochemical Hydrogen Evolution

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Coupling NiSe₂ Nanoparticles with N-Doped Porous Carbon Enables Efficient and Durable Electrocatalytic Hydrogen Evolution Reaction at pH Values Ranging from 0 to 14

Coupling NiSe₂ Nanoparticles with N-Doped Porous Carbon Enables Efficient and Durable Electrocatalytic Hydrogen Evolution Reaction at pH Values Ranging from 0 to 14