Mesoporous carbon nitride supported 5,10,15,20-tetrakis(4-methoxyphenyl)-21H,23H-porphine cobalt(<scp>ii</scp>) as a selective and durable electrocatalyst for the production of hydrogen peroxide via two-electron oxygen reduction

Singh, Devesh Kumar; Ganesan, Vellaichamy; Yadav, Dharmendra Kumar; Yadav, Mamta; Sonkar, Piyush Kumar; Gupta, Rupali

doi:10.1039/d0cy01801e

Cited by 18 publications

(19 citation statements)

References 79 publications

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“…Since H 2 O 2 is a reaction intermediate in ORR, it can (under certain conditions) be the final product of a two-electron reduction process [ 5 , 6 , 7 ]. Ideally, the catalysts for ORR should be active for the HPRR.…”

Section: Introductionmentioning

confidence: 99%

Facile Synthesis of Low-Cost Copper-Silver and Cobalt-Silver Alloy Nanoparticles on Reduced Graphene Oxide as Efficient Electrocatalysts for Oxygen Reduction Reaction in Alkaline Media

et al. 2022

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Copper-silver and cobalt-silver alloy nanoparticles deposited on reduced graphene oxide (CuAg/rGO and CoAg/rGO) were synthesized and examined as electrocatalysts for oxygen reduction reaction (ORR) and hydrogen peroxide reduction reaction (HPRR) in alkaline media. Characterization of the prepared samples was done by transmission electron microscopy (TEM), Fourier-transform infrared spectroscopy (FTIR), Raman spectroscopy, X-ray diffraction analysis (XRD), and scanning electron microscopy with integrated energy-dispersive X-ray spectroscopy (SEM-EDS). CuAg/rGO and CoAg/rGO nanoparticles diameter ranged from 0.4 to 9.2 nm. The Ag loading was ca. 40 wt.% for both electrocatalysts, with that for Cu and Co being 35 and 17 wt.%, respectively. CoAg/rGO electrocatalyst showed a Tafel slope of 109 mV dec−1, significantly lower than that for CuAg/rGO (184 mV dec−1), suggesting faster ORR kinetics. Additionally, a higher diffusion current density was obtained for CoAg/rGO (−2.63 mA cm−2) than for CuAg/rGO (−1.74 mA cm−2). The average value of the number of electrons transferred during ORR was 2.8 for CuAg/rGO and 3.3 for CoAg/rGO electrocatalyst, further confirming the higher ORR activity of the latter. On the other hand, CuAg/rGO showed higher peak current densities (−3.96 mA cm−2) for HPRR compared to those recorded for CoAg/rGO electrocatalyst (−1.96 mA cm−2).

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Section: Introductionmentioning

confidence: 99%

Facile Synthesis of Low-Cost Copper-Silver and Cobalt-Silver Alloy Nanoparticles on Reduced Graphene Oxide as Efficient Electrocatalysts for Oxygen Reduction Reaction in Alkaline Media

et al. 2022

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“…The atomic ratio of each element and the ratio of chemical bonds are shown in Tables S1−S5. For the N 1s spectra (Figure 3d), four peaks at approximately 398.47, 399.16, 400.66, and 401.31 eV correspond to pyridinic N, Cr−N, pyrrolic N, and graphitic N. 22,40 The presence of the Cr−N bond in Cr-ABIm and Cr-ABIm@BP2000 showed that the Cr atom is embedded in the building blocks of the mixture through the stable coordination bond mode. The Cr 2p 1/2 peak is located at about 586.7 eV (Figure 3e).…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…The electrochemical active area (ECSA) of the catalyst was derived from the electrochemical double-layer capacitance (C dl ). The capacitance current of the double layer in the non-Faraday interval corresponding to the cyclic voltammetry curve at different sweep speeds (20,40,60,80, and 100 mV s −1 ) was measured. At 0.125 vs RHE, C dl can be obtained from a function of disk current density and scan rates.…”

Section: ■ Experimental Methodsmentioning

confidence: 99%

Valence State Modulation of Chromium in Selective Hydrogen Peroxide Production Electrocatalysts

Zhang

Wang

et al. 2021

ACS Appl. Energy Mater.

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Hydrogen peroxide (H 2 O 2 ) is a worthy chemical substance with comprehensive applications, but its practical industrial methods involve complex and energy-consuming procedures. Electrocatalytic oxygen reduction for the production of H 2 O 2 is a flexible alternative strategy, which requires a low-cost catalyst with high activity and selectivity for the 2e − ORR pathway. Here, we first present a straightforward and universal one-step hydrothermal method that directly combines Cr-ABIm with commercial carbon black (BP2000) to prepare H 2 O 2 electrochemically with high selectivity and energy saving. A variety of characterization analyses display that the introduction of Cr-ABIm increases the number of defects and active sites and also enlarges the surface area of the catalyst for electrochemical reactions. Importantly, the valence state of Cr is changed (Cr 3+ of Cr-ABIm converted to Cr 5+ ) when Cr-ABIm anchors on BP2000, which accelerates the activity of the reduction reaction. The selectivity of the catalyst for H 2 O 2 preparation is also determined by Koutecky−Levich analysis and rotating ring disk electrochemical tests. In a potential range of 0.2−0.7 V (vs reversible hydrogen electrode (RHE)), the electron transfer number of the Cr-ABIm@BP2000 catalyst is on the verge of 2.5, and the electrogenerated yield of H 2 O 2 is 65%. In addition, its mass activity at 0.5 V is up to 7.56 A g −1 . Density functional theory (DFT) calculations clarify that suitable N, O coordination on the active surface of BP2000s acquires the changing capacity of the valence state of Cr, thereby regulating the adsorption of intermediate products and endowing it with superior H 2 O 2 performance. It is believed that Cr-ABIm@ BP2000 will be a viable electrocatalyst for sustainable in situ generation of H 2 O 2 from oxygen.

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“…Mesoporous carbon nitride (MCN) has been evaluated as a support for both metal (Mn, Fe, Co, Ni, Cu, and Zn) phthalocyanine and Co porphyrin ORR catalysts by Singh et al , The MCN was synthesized by a hard templating method to improve the surface area and conductivity of the support. The highest E 1/2 (∼0.05 V) is exhibited by CoPc@MCN in these reports, with a limiting current density < 1.5 mA/cm 2 and n ∼ 1.64 in 0.1 M HClO 4 with rotation.…”

Section: Introductionmentioning

confidence: 99%

Effect of Support on Oxygen Reduction Reaction Activity of Supported Iron Porphyrins

et al. 2022

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We report the oxygen reduction reaction (ORR) activity in acid of an Fe porphyrin on different supports. While the activity is high (E 1/2 = 0.34 V vs RHE with n = 3.8) when the Fe porphyrin is adsorbed on XC72 (a graphitic carbon), this activity is much lower when the porphyrin is adsorbed on either MoS 2 (E 1/2 = −0.15 V vs RHE with n = 2.2) or g-C 3 N 4 (E 1/2 = −0.24 V vs RHE with n = 3.1). Electron paramagnetic resonance (EPR), X-ray absorption fine structure (XAFS), and magnetometry measurements show the electronic structure around the Fe center is the same for all three supports. Only the Fe porphyrin supported on XC72 exhibits a pH dependence in its ORR activity. This observation, coupled with the increased hydrophilicity of XC72 relative to the other supports, suggests that the support-electrolyte interaction controls the ORR activity. Modification of MoS 2 to increase its hydrophilicity results in a more active ORR catalyst.

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Mesoporous carbon nitride supported 5,10,15,20-tetrakis(4-methoxyphenyl)-21H,23H-porphine cobalt(ii) as a selective and durable electrocatalyst for the production of hydrogen peroxide via two-electron oxygen reduction

Cited by 18 publications

References 79 publications

Facile Synthesis of Low-Cost Copper-Silver and Cobalt-Silver Alloy Nanoparticles on Reduced Graphene Oxide as Efficient Electrocatalysts for Oxygen Reduction Reaction in Alkaline Media

Facile Synthesis of Low-Cost Copper-Silver and Cobalt-Silver Alloy Nanoparticles on Reduced Graphene Oxide as Efficient Electrocatalysts for Oxygen Reduction Reaction in Alkaline Media

Valence State Modulation of Chromium in Selective Hydrogen Peroxide Production Electrocatalysts

Effect of Support on Oxygen Reduction Reaction Activity of Supported Iron Porphyrins

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