Heterogeneous Co–N/C Electrocatalysts with Controlled Cobalt Site Densities for the Hydrogen Evolution Reaction: Structure–Activity Correlations and Kinetic Insights

ACS Catalysis ◽  
2018 ◽  
Vol 9 (1) ◽  
pp. 83-97 ◽  
Author(s):  
Young Jin Sa ◽  
Sung O Park ◽  
Gwan Yeong Jung ◽  
Tae Joo Shin ◽  
Hu Young Jeong ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
Structure Activity

scholarly journals Electronic metal–support interaction modulates single-atom platinum catalysis for hydrogen evolution reaction

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Yi Shi ◽  
Zhi-Rui Ma ◽  
Yi-Ying Xiao ◽  
Yun-Chao Yin ◽  
Wen-Mao Huang ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
Structure Activity Relationship ◽  
Atomic Level ◽  
Single Atom ◽  
Activity Relationship ◽  
Support Interaction ◽  
Structure Activity ◽  
Metal Support Interaction ◽  
Metal Support

AbstractTuning metal–support interaction has been considered as an effective approach to modulate the electronic structure and catalytic activity of supported metal catalysts. At the atomic level, the understanding of the structure–activity relationship still remains obscure in heterogeneous catalysis, such as the conversion of water (alkaline) or hydronium ions (acid) to hydrogen (hydrogen evolution reaction, HER). Here, we reveal that the fine control over the oxidation states of single-atom Pt catalysts through electronic metal–support interaction significantly modulates the catalytic activities in either acidic or alkaline HER. Combined with detailed spectroscopic and electrochemical characterizations, the structure–activity relationship is established by correlating the acidic/alkaline HER activity with the average oxidation state of single-atom Pt and the Pt–H/Pt–OH interaction. This study sheds light on the atomic-level mechanistic understanding of acidic and alkaline HER, and further provides guidelines for the rational design of high-performance single-atom catalysts.

scholarly journals Theoretical evaluation of the structure–activity relationship in graphene-based electrocatalysts for hydrogen evolution reactions

RSC Advances ◽  
2017 ◽  
Vol 7 (43) ◽  
pp. 27033-27039 ◽  
Author(s):  
Chi Ho Lee ◽  
Byeongsun Jun ◽  
Sang Uck Lee
Keyword(s):  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
Electrocatalytic Activity ◽  
Structure Activity Relationship ◽  
Activity Relationship ◽  
Theoretical Evaluation ◽  
Structure Activity ◽  
Hydrogen Evolution Reactions ◽  
The Relationship

We systematically analyzed the relationship between structure and electrocatalytic activity of heteroatom-doped graphenes (GXs, where G and X represent graphene and the heteroatom dopant) for the hydrogen evolution reaction (HER).

scholarly journals Increasing the rate of the hydrogen evolution reaction in neutral water with protic buffer electrolytes

2020 ◽  
Vol 117 (52) ◽  
pp. 32947-32953
Author(s):  
Kayla E. Clary ◽  
Metin Karayilan ◽  
Keelee C. McCleary-Petersen ◽  
Haley A. Petersen ◽  
Richard S. Glass ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
Sodium Phosphate ◽  
Primary Source ◽  
Phosphate Solution ◽  
Catalytic Current ◽  
Structure Activity ◽  
Proton Source ◽  
Sodium Phosphate Solution ◽  
Current Densities

Electrocatalytic generation of H2 is challenging in neutral pH water, where high catalytic currents for the hydrogen evolution reaction (HER) are particularly sensitive to the proton source and solution characteristics. A tris(hydroxymethyl)aminomethane (TRIS) solution at pH 7 with a [2Fe-2S]-metallopolymer electrocatalyst gave catalytic current densities around two orders of magnitude greater than either a more conventional sodium phosphate solution or a potassium chloride (KCl) electrolyte solution. For a planar polycrystalline Pt disk electrode, a TRIS solution at pH 7 increased the catalytic current densities for H2 generation by 50 mA/cm2 at current densities over 100 mA/cm2 compared to a sodium phosphate solution. As a special feature of this study, TRIS is acting not only as the primary source of protons and the buffer of the pH, but the protonated TRIS ([TRIS-H]+) is also the sole cation of the electrolyte. A species that is simultaneously the proton source, buffer, and sole electrolyte is termed a protic buffer electrolyte (PBE). The structure–activity relationships of the TRIS PBE that increase the HER rate of the metallopolymer and platinum catalysts are discussed. These results suggest that appropriately designed PBEs can improve HER rates of any homogeneous or heterogeneous electrocatalyst system. General guidelines for selecting a PBE to improve the catalytic current density of HER systems are offered.

Sequential self-reconstruction of localized Mo species in hierarchical carbon/Co–Mo oxide heterostructures for boosting alkaline hydrogen evolution kinetics and durability

2022 ◽  
Author(s):  
Quan Quan ◽  
Xiuming Bu ◽  
Dong Chen ◽  
Fei Wang ◽  
Xiaolin Kang ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
Oxide Heterostructures ◽  
Structure Activity Relationships ◽  
Structure Activity ◽  
Localized Mo ◽  
Hierarchical Carbon

Surface self-reconstruction processes in alkaline hydrogen evolution reaction (HER), especially regarding the explicit structure-activity relationships, remain elusive. Here, we first design a hierarchical Co@NCNT/CoMoOx precatalyst constituted by the defective CoMoOx...

A crystalline–amorphous Ni–Ni(OH)2 core–shell catalyst for the alkaline hydrogen evolution reaction

2020 ◽  
Vol 8 (44) ◽  
pp. 23323-23329
Author(s):  
Jing Hu ◽  
Siwei Li ◽  
Yuzhi Li ◽  
Jing Wang ◽  
Yunchen Du ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
Electrocatalytic Activity ◽  
Core Shell ◽  
Alkaline Conditions

Crystalline–amorphous Ni–Ni(OH)2 core–shell assembled nanosheets exhibit outstanding electrocatalytic activity and stability for hydrogen evolution under alkaline conditions.

Cobaloxime-Based Double Complex Salts as Efficient and Versatile Catalysts for the Light-Driven Hydrogen Evolution Reaction

2020 ◽  
Author(s):  
Elisabeth Hofmeister ◽  
Jisoo Woo ◽  
Tobias Ullrich ◽  
Lydia Petermann ◽  
Kevin Hanus ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
Systematic Study ◽  
Cobalt Complexes ◽  
Spectroscopic Studies ◽  
Double Complex ◽  
Double Complex Salts ◽  
Noble Metal Catalysts ◽  
Reduction Potentials ◽  
Complex Salts

Cobaloximes and their BF<sub>2</sub>-bridged analogues have emerged as promising non-noble metal catalysts for the photocatalytic hydrogen evolution reaction (HER). Herein we report the serendipitous discovery that double complex salts such as [Co(dmgh)<sub>2</sub>py<sub>2</sub>]<sup>+</sup>[Co(dmgBPh<sub>2</sub>)<sub>2</sub>Cl<sub>2</sub>]<sup>-</sup> can be obtained in good yields by treatment of commercially available [Co(dmgh)<sub>2</sub>pyCl] with triarylboranes. A systematic study on the use of such double complex salts and their single salts with simple counterions as photocatalysts revealed HER activities comparable or superior to existing cobaloxime catalysts and suggests ample opportunities for this compound class in catalyst/photosensitizer dyads and immobilized architectures. Preliminary electrochemical and spectroscopic studies indicate that one key advantage of these charged cobalt complexes is that the reduction potentials as well as the electrostatic interaction with charged photosensitizers can be tuned.

2,2’-Dipyridylamine as Organic Molecular Electrocatalyst for Hydrogen Evolution Reaction in Acidic Electrolytes

2019 ◽  
Author(s):  
Xi Yin ◽  
Ling Lin ◽  
Hoon T. Chung ◽  
Ulises Martinez ◽  
Andrew M. Baker ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
Density Functional ◽  
Low Cost ◽  
Membrane Electrode Assembly ◽  
Carbon Surface ◽  
Membrane Electrode ◽  
Durability Test ◽  
Onset Potential ◽  
Precious Metal Catalysts

Finding a low-cost and stable electrocatalyst for hydrogen evolution reaction (HER) as a replacement for scarce and expensive precious metal catalysts has attracted significant interest from chemical and materials research communities. Here, we demonstrate an organic catalyst based on 2,2’-dipyridylamine (dpa) molecules adsorbed on carbon surface, which shows remarkable hydrogen evolution activity and performance durability in strongly acidic polymer electrolytes without involving any metal. The HER onset potential at dpa adsorbed on carbon has been found to be less than 50 mV in sulfuric acid and in a Nafion-based membrane electrode assembly (MEA). At the same time, this catalyst has shown no performance loss in a 60-hour durability test. The HER reaction mechanisms and the low onset overpotential in this system are revealed based on electrochemical study. Density functional theory (DFT) calculations suggest that the pyridyl-N functions as the active site for H adsorption with a free energy of -0.13 eV, in agreement with the unusually low onset overpotential for an organic molecular catalyst.<br>

2,2’-Dipyridylamine as Organic Molecular Electrocatalyst for Hydrogen Evolution Reaction in Acidic Electrolytes

2019 ◽  
Author(s):  
Xi Yin ◽  
Ling Lin ◽  
Hoon T. Chung ◽  
Ulises Martinez ◽  
Andrew M. Baker ◽  
...  
Keyword(s):  
Hydrogen Evolution ◽  
Hydrogen Evolution Reaction ◽  
Density Functional ◽  
Low Cost ◽  
Membrane Electrode Assembly ◽  
Carbon Surface ◽  
Membrane Electrode ◽  
Durability Test ◽  
Onset Potential ◽  
Precious Metal Catalysts

Finding a low-cost and stable electrocatalyst for hydrogen evolution reaction (HER) as a replacement for scarce and expensive precious metal catalysts has attracted significant interest from chemical and materials research communities. Here, we demonstrate an organic catalyst based on 2,2’-dipyridylamine (dpa) molecules adsorbed on carbon surface, which shows remarkable hydrogen evolution activity and performance durability in strongly acidic polymer electrolytes without involving any metal. The HER onset potential at dpa adsorbed on carbon has been found to be less than 50 mV in sulfuric acid and in a Nafion-based membrane electrode assembly (MEA). At the same time, this catalyst has shown no performance loss in a 60-hour durability test. The HER reaction mechanisms and the low onset overpotential in this system are revealed based on electrochemical study. Density functional theory (DFT) calculations suggest that the pyridyl-N functions as the active site for H adsorption with a free energy of -0.13 eV, in agreement with the unusually low onset overpotential for an organic molecular catalyst.<br>

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