“…[ 10 ] The spatial isolation of metal atoms can modulate the adsorption energy for reaction substrates and intermediates, thereby accelerate the reaction process. [ 11 ]…”
The electrosynthesis from 5‐hydroxymethylfurfural (HMF) is considered a green strategy to achieve biomass‐derived high‐value chemicals. As the molecular structure of HMF is relatively complicated, understanding the HMF adsorption/catalysis behavior on electrocatalysts is vital for biomass‐based electrosynthesis. The electrocatalysis behavior can be modulated by tuning the adsorption energy of the reactive molecules. In this work, the HMF adsorption behavior on spinel oxide, Co3O4 is discovered. Correspondingly, the adsorption energy of HMF on Co3O4 is successfully tuned by decorating with single‐atom Ir. It is observed that compared with bare Co3O4, single‐atom‐Ir‐loaded Co3O4 (Ir‐Co3O4) can enhance adsorption with the CC groups of HMF. The synergetic adsorption can enhance the overall conversion of HMF on electrocatalysts. With the modulated HMF adsorption, the as‐designed Ir‐Co3O4 exhibits a record performance (with an onset potential of 1.15 VRHE) for the electrosynthesis from HMF.
“…[ 10 ] The spatial isolation of metal atoms can modulate the adsorption energy for reaction substrates and intermediates, thereby accelerate the reaction process. [ 11 ]…”
The electrosynthesis from 5‐hydroxymethylfurfural (HMF) is considered a green strategy to achieve biomass‐derived high‐value chemicals. As the molecular structure of HMF is relatively complicated, understanding the HMF adsorption/catalysis behavior on electrocatalysts is vital for biomass‐based electrosynthesis. The electrocatalysis behavior can be modulated by tuning the adsorption energy of the reactive molecules. In this work, the HMF adsorption behavior on spinel oxide, Co3O4 is discovered. Correspondingly, the adsorption energy of HMF on Co3O4 is successfully tuned by decorating with single‐atom Ir. It is observed that compared with bare Co3O4, single‐atom‐Ir‐loaded Co3O4 (Ir‐Co3O4) can enhance adsorption with the CC groups of HMF. The synergetic adsorption can enhance the overall conversion of HMF on electrocatalysts. With the modulated HMF adsorption, the as‐designed Ir‐Co3O4 exhibits a record performance (with an onset potential of 1.15 VRHE) for the electrosynthesis from HMF.
“…Wang and coworkers used a general strategy of host–guest ( Figure a), which synthesized a series of N‐doped carbon‐based SAM (denoted as M1/CN, M = Pt, Pd, Ir, Mo, Ru, Cu, Ga, Mn, Ni) toward the formic acid oxidation reaction (FAOR). [ 22 ] Among these TE, the Ir1/CN exhibits high activity during the FAOR. Compared with the inert Ir nanoparticles supported by carbon, the valence state of the Ir δ+ in IrN 4 is more positive than that of Ir nanoparticles, which leads to a more vacancy of d‐orbital in IrN 4 and weaker back‐donation interaction.…”
Section: How To Regulate the Structure Of Sam?mentioning
confidence: 99%
“…Reproduced with permission. [ 22 ] Copyright 2020, Springer Nature. b) Gibbs free energy diagram of the FAOR on Ir1/CN.…”
Section: How To Regulate the Structure Of Sam?mentioning
confidence: 99%
“…Reproduced with permission. [ 22 ] Copyright 2020, Springer Nature. c) Schematic of the preparation strategy for SA‐Rh/CN.…”
Section: How To Regulate the Structure Of Sam?mentioning
Single‐atom materials (SAMs) have been widely investigated during the past years, providing many high‐performance materials applied in catalyst, battery, solar cell, and so on. The high performance that SAM exhibit is largely attributed to the microstructure inside the SAM. It is thus essential to realize the goal of regulating the structures, as the chemists wish and deeply comprehend the relationship between the macroproperties and the small structures. However, the concerns above are far from realization and more efforts are necessary to be put into this field. Herein, the regulation on microstructures, the characterization on the microstructures and the relationship between the macroproperties and the small structures are comprehensively summarized and discussed, which are mainly based on the application of SAM in catalyst. Based on the basic information earlier, the challenge and future development of SAM are also proposed, aiming to emerge an overall view and guideline to the research on the next step.
“…Sub-nanosized metal clusters and nanoparticles usually possess higher catalytic activity and selectivity as compared with bulk metal [19][20][21][22]. As an effective approach to lower the cost and consumption of catalysts, single-atom catalysts (SACs), which was first proposed in 2011 [23][24][25][26], have become promising alternative in heterogeneous catalysis [27][28][29][30]. SACs embedded on different supports have revealed superb catalytic activity and selectivity as compared with subnanosized metal clusters [31,32].…”
MXene is a variety of new two-dimensional (2D) materials with early transition metal carbides, nitrides, and carbonitrides. Quantum chemical studies have been carried out on the geometries, electronic structures, stability and catalytic properties of a non-noble metal single-atom catalyst (SAC) with single Co atom anchored on MXene materials of Mo 2 CS 2. The Co adatom anchored on top of the Mo atom of this MXene is found to be rather stable, and this SAC is appropriate for CO oxidation. The charge transfers from the surface to the adsorbed CO and O 2 play a significant role in the activation of these molecules on Co 1 /Mo 2 CS 2. With this catalyst, the Eley-Rideal (ER), Langmuir-Hinshelwood (LH), and Termolecular Eley-Rideal (TER) mechanisms are explored for CO oxidation. We find that, while all the three mechanisms are feasible at low temperature, Co 1 /Mo 2 CS 2 possesses higher catalytic activity for CO oxidation through the TER mechanism that features an intriguing OC(OO)CO intermediate (IM) adsorbed on Co single atom. The calculated activation energy barriers of the rate-limiting step are 0.67 eV (TER), 0.78 eV (LH) and 0.88 eV (ER), respectively. The present study illustrates that it is promising to develop and design low-cost, non-noble metal SACs using MXene types of 2D materials.
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