The reformation of catalyst: From a trial-and-error synthesis to rational design

Wang, Ligang; Wu, Jiabin; Wang, Shunwu; Liu, Huan; Wang, Yao; Wang, Dingsheng

doi:10.1007/s12274-023-6037-8

Cited by 151 publications

(47 citation statements)

References 388 publications

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“…In the multielectrons involved reaction, the cluster/nanoparticles material may perform higher efficiency. [62][63][64][65][66][67] Therefore, it is essential to clarify the difference between these two types of materials. As the active sites are dispersed as a single atom, the sites and status for reactants adsorbing on SAMs are usually simple and unitary, which results in high selectivity in many reactions (e.g., CO 2 RR and some organic synthesis) and sometimes high efficiency towards some singleelectron transfer reaction.…”

Section: Discussionmentioning

confidence: 99%

“…Electrocatalysis is one of the hottest topics in the field of chemistry, including fuel cells, electro-organic synthesis, water overall splitting, and so on. [61][62][63][64] With the development of SAM, there are many exciting results in this field, indicating the important role of SAM in the conversion of electricity.…”

Section: Conversion Between Electricity and Chemical Energymentioning

confidence: 99%

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Single‐atom materials: The application in energy conversion

Zhu,

Yang,

Zhang

et al. 2024

Interdisciplinary Materials

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Single‐atom materials (SAMs) have become one of the most important power sources to push the field of energy conversion forward. Among the main types of energy, including thermal energy, electrical energy, solar energy, and biomass energy, SAMs have realized ultra‐high efficiency and show an appealing future in practical application. More than high activity, the uniform active sites also provide a convincible model for chemists to design and comprehend the mechanism behind the phenomenon. Therefore, we presented an insightful review of the application of the single‐atom material in the field of energy conversion. The challenges (e.g., accurate synthesis and practical application) and future directions (e.g., machine learning and efficient design) of the applications of SAMs in energy conversion are included, aiming to provide guidance for the research in the next step.

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Section: Discussionmentioning

confidence: 99%

Section: Conversion Between Electricity and Chemical Energymentioning

confidence: 99%

Single‐atom materials: The application in energy conversion

Zhu,

Yang,

Zhang

et al. 2024

Interdisciplinary Materials

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“…Single-atom catalysts (SACs) have attracted wide attention due to their maximum atomic utilization and unique electronic and spatial structure. − Varieties of successful strategies have been developed for the preparation of SACs. , Among them, the direct pyrolysis of metal-zeolite imidazolate frameworks (M-ZIFs) currently stands as the predominant method for the preparation of atomically dispersed metal–nitrogen-carbon SACs (M/NC-SACs). − The catalysts synthesized using this approach have demonstrated remarkable efficiency in catalyzing the semihydrogenation of alkynes. ,− For example, our recent study demonstrated that the Pd-NC catalyst enabled the efficient semihydrogenation of acetylene . However, when dealing with larger molecules such as phenylacetylene, the narrow pore structure inherent in ZIF-derived catalysts restricted molecular diffusion and diminished the utilization rate of internal active sites, and consequently led to reduced catalyst activity. − Liu and Han et al developed a facile topo-conversion strategy to fabricate hollow mesoporous M/NC-SACs with enhanced diffusion properties for catalysis .…”

Section: Introductionmentioning

confidence: 99%

Pd–Mn/NC Dual Single-Atomic Sites with Hollow Mesopores for the Highly Efficient Semihydrogenation of Phenylacetylene

Liu,

Zhu,

Yang

et al. 2024

J. Am. Chem. Soc.

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The direct pyrolysis of metal-zeolite imidazolate frameworks (M-ZIFs) has been widely recognized as the predominant approach for synthesizing atomically dispersed metal−nitrogen-carbon single-atom catalysts (M/NC-SACs), which have exhibited exceptional activity and selectivity in the semihydrogenation of acetylene. However, due to weak adsorption of reactants on the single site and restricted molecular diffusion, the semihydrogenation of large organic molecules (e.g., phenylacetylene) was greatly limited for M/NC-SACs. In this work, a dual single-atom catalyst (h−Pd-Mn/NC) with hollow mesopores was designed and prepared using a general host−guest strategy. Taking the semihydrogenation of phenylacetylene as an example, this catalyst exhibited ultrahigh activity and selectivity, which achieved a turnover frequency of 218 mol C�C mol Pd −1 min −1 , 16-fold higher than that of the commercial Lindlar catalyst. The catalyst maintained high activity and selectivity even after 5 cycles of usage. The superior activity of h−Pd-Mn/NC was attributed to the 4.0 nm mesopore interface of the catalyst, which enhanced the diffusion of macromolecular reactants and products. Particularly, the introduction of atomically dispersed Mn with weak electronegativity in h−Pd-Mn/NC could drive the electron transfer from Mn to adjacent Pd sites and regulate the electronic structure of Pd sites. Meanwhile, the strong electronic coupling in Pd−Mn pairs enhanced the d-electron domination near the Fermi level and promoted the adsorption of phenylacetylene and H 2 on Pd active sites, thereby reducing the energy barrier for the semihydrogenation of phenylacetylene.

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“…The high cost, toxicity, and easy CO poison restrict their further applications . Efficient catalysts can accelerate reaction rates and promote the effective conversion of molecules, which is of great significance in chemical engineering, energy, materials, and the environment. , …”

Section: Introductionmentioning

confidence: 99%

Coordination Confined Thermolysis Synthesis of the Ni Single Atom Catalyst on the N-Doped Commercial Carbon for the Production of Syngas

Chen,

Shen,

Dai

et al. 2024

Inorg. Chem.

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The electrochemical conversion of CO 2 into controllable syngas (CO/H 2 ) over a wide potential range is challenging. The main electrocatalysts are based on the noble metals Au (Ag) or heavy metal Pb. The development of alternative nonprecious catalysts is of paramount importance for practice. In this work, a simple coordination confined thermal pyrolysis method has been developed for the synthesis of Ni single-atom catalyst loaded onto nitrogen-doped commercial carbon. The catalyst is in the form of NiN 3 −C, which exhibits a high-performance electrocatalytic reduction of CO 2 toward producing syngas with Faraday efficiencies of 62.28% of CO and 36.7% of H 2 . The Gibbs free energies of COOH* and H* on the NiN 3 −C structure were estimated by using density functional theory (DFT). The formation of COOH* intermediate is the speed-limiting step in the process, with ΔG COOH* being 0.7 eV, while H* is the speed-limiting step in the hydrogen evolution, respectively. This work provides a feasible method for the achievement of nonprecious catalysts for the resourceful use of CO 2 .

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The reformation of catalyst: From a trial-and-error synthesis to rational design

Cited by 151 publications

References 388 publications

Single‐atom materials: The application in energy conversion

Single‐atom materials: The application in energy conversion

Pd–Mn/NC Dual Single-Atomic Sites with Hollow Mesopores for the Highly Efficient Semihydrogenation of Phenylacetylene

Coordination Confined Thermolysis Synthesis of the Ni Single Atom Catalyst on the N-Doped Commercial Carbon for the Production of Syngas

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