Single‐Atom Catalysts for the Hydrogen Evolution Reaction

Liu, Haoxuan; Peng, Xianyun; Liu, Xijun

doi:10.1002/celc.201800507

Cited by 98 publications

(60 citation statements)

References 130 publications

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“…Electrochemical water splitting through HER provides a sustainable and green route to produce molecular hydrogen (H 2 ) for mitigating the global energy crisis; however, the development of active catalysts with minimal overpotential and high efficiency is still urgently demanded for its large-scale application. Recently, SACs supported on various kinds of materials including MoS 2 , MXene, and carbon-based matrix have been widely used to catalyze HER (108)(109)(110). Microenvironment engineering of atomically dispersed active sites, which can result in unique structures and electronic properties of SACs, has been proven as a promising way to dramatically accelerate the reaction kinetics of HER.…”

Section: Hydrogen Evolution Reactionmentioning

confidence: 99%

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

et al. 2020

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Single-atom catalysts (SACs) have become the most attractive frontier research field in heterogeneous catalysis. Since the atomically dispersed metal atoms are commonly stabilized by ionic/covalent interactions with neighboring atoms, the geometric and electronic structures of SACs depend greatly on their microenvironment, which, in turn, determine the performances in catalytic processes. In this review, we will focus on the recently developed strategies of SAC synthesis, with attention on the microenvironment modulation of single-atom active sites of SACs. Furthermore, experimental and computational advances in understanding such microenvironment in association to the catalytic activity and mechanisms are summarized and exemplified in the electrochemical applications, including the water electrolysis and O2/CO2/N2 reduction reactions. Last, by highlighting the prospects and challenges for microenvironment engineering of SACs, we wish to shed some light on the further development of SACs for electrochemical energy conversion.

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Section: Hydrogen Evolution Reactionmentioning

confidence: 99%

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

et al. 2020

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“…H + + e -→Had (Volmer step in an acid solution) [148] *N-CNTs, N-doped C nanotubes; HMS, hollow microsphere; GC, glassy C; NCV, N-doped C vesicle; NC, ultrathin graphene shells (only 1-3 layers); NPA, nanoplate arrays; NGF, N-doped graphene foam; PC, porous carbon; CP, C paper; HNW, hybrid nanowire; BHSs, double-shelled hollow nanospheres; CC, C cloth; NF, Ni foam; CF, C fiber; NPC, nanoporous Cu. H2O+ e -→Had + OH -(Volmer step in an alkaline solution, 120 mV dec -1 ) (2) Had + Had → H2 (Tafel, 30 mV dec -1 ) (3) H + + Had + e -→ H2 (Heyrovsky) (4) H2O+ Had + e -→ H2 + OH -(Heyrovsky, 40 mV dec -1 ) (5) Moreover, to further enhance the activity and stability of these H2-evolution electrocatalysts, five designing strategies have been developed, namely composition engineering, [149][150][151][152][153][154][155][156][157] nanostructure engineering [158][159][160][161][162][163][164][165][166][167], interfacial engineering [168][169][170][171][172][173][174], surface engineering, [175], and hybrid engineering [176][177][178][179][180][181] (Fig. 5).…”

Section: Fundamentals Of Ni-based H2-production Electrocatalystsmentioning

confidence: 99%

Ni-based photocatalytic H2-production cocatalysts2

Shen

Xie

Xiang

et al. 2019

Chinese Journal of Catalysis

256

108

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Photocatalysis is believed to be one of the best methods to realize sustainable H2 production. However, achieving this through heterogeneous photocatalysis still remains a great challenge owing to the absence of active sites, sluggish surface reaction kinetics, insufficient charge separation, and a high thermodynamic barrier. Therefore, cocatalysts are necessary and of great significance in boosting photocatalytic H2 generation. This review will focus on the promising and appealing low-cost Ni-based H2-generation cocatalysts as the alternatives for the high-cost and low-abundance noble metal cocatalysts. Special emphasis has been placed on the design principle, modification strategies for further enhancing the activity and stability of Ni-based cocatalysts, and identification of the exact active sites and surface reaction mechanisms. Particularly, four types of modification strategies based on increased light harvesting, enhanced charge separation, strengthened interface interaction, and improved electrocatalytic activity have been thoroughly discussed and compared in detail. This review may open a new avenue for designing highly active and durable Ni-based cocatalysts for photocatalytic H2 generation.

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“…[ 3 ] The major unexposed metal atoms in the bulk phase are inert for HER, which strictly limits the metal atom utilization. [ 4–6 ]…”

Section: Introductionmentioning

confidence: 99%

Conductive Metal–Organic Frameworks with Extra Metallic Sites as an Efficient Electrocatalyst for the Hydrogen Evolution Reaction

et al. 2020

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The 2D conductive metal–organic frameworks (MOFs) are expected to be an ideal electrocatalyst due to their high utilization of metal atoms. Exploring a new conjugated ligand with extra active metallic center can further boost the structural advantages of conductive MOFs. In this work, hexaiminohexaazatrinaphthalene (HAHATN) is employed as a conjugated ligand to construct bimetallic sited conductive MOFs (M23(M13∙HAHATN)2) with an extra M–N2 moiety. Density functional theory (DFT) calculations demonstrate that the 2D conjugated framework renders M23(M13∙HAHATN)2 a high electric conductivity with narrow bandgap (0.19 eV) for electron transfer and a favorable in‐plane porous structure (2.7 nm) for mass transfer. Moreover, the metal atom at the extra M–N2 moiety has a higher unsaturation degree than that at M–N4 linkage, resulting in a stronger ability to donate electrons for enhancing electroactivity. These characteristics endow the new conductive MOFs with an enhanced electroactivity for hydrogen evolution reaction (HER) electrocatalysis. Among the series of M23(M13∙HAHATN)2 MOF, Ni3(Ni3∙HAHATN)2 nanosheets with the optimal structure exhibit a small overpotential of 115 mV at 10 mA cm−2, low Tafel slope of (45.6 mV dec−1), and promising electrocatalytic stability for HER. This work provides an effective strategy for designing conductive MOFs with a favorable structure for electrocatalysis.

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Single‐Atom Catalysts for the Hydrogen Evolution Reaction

Cited by 98 publications

References 130 publications

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Ni-based photocatalytic H2-production cocatalysts2

Conductive Metal–Organic Frameworks with Extra Metallic Sites as an Efficient Electrocatalyst for the Hydrogen Evolution Reaction

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