N, O-dual coordination regulation directs the design of active sites on nanoclusters for highly efficient catalytic water purification

Dai, Fangfang; Xie, Mingsen; Wang, Shuoxuan; Lv, Weiqiang; Wang, Yong; Zhang, Zhen; Lu, Xiaoquan

doi:10.1016/j.apcatb.2023.122510

Cited by 14 publications

(3 citation statements)

References 56 publications

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“…In these materials, the EMSI via the electrons transferred between the metal and support can stabilize the metallic species and modulate their electronic structures by causing substantial electronic perturbations and redistributing the charge density of the active sites. [42][43][44][45] Therefore, tailoring the EMSI via rational coordination of the metallic species is expected to be an effective and versatile way to create Lewis acid sites for exclusive NRR active mode, which though is still rarely reported.…”

Section: Introductionmentioning

confidence: 99%

Improving Electrocatalytic Nitrogen Reduction Selectivity and Yield by Suppressing Hydrogen Evolution Reaction via Electronic Metal–Support Interaction

Xie

Dai

Guo

et al. 2023

Advanced Energy Materials

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the H 2 precursor. This energy-intensive process reportedly costs ≈1.5% of the annual global energy consumption. [1,2] The electrocatalytic N 2 reduction reaction (NRR), which uses a renewable energy source and N 2 and H 2 O as the reactants, presents a highly promising strategy for NH 3 production under ambient conditions. [3][4][5][6][7] However, two aspects: poor catalytic activity and low selectivity of the electrocatalyst, significantly restrict the NRR process. First, the inert nitrogen with high cleavage energy (940.95 kJ mol −1 ) has sluggish adsorption on the catalysts, owing to the lack of active sites on the catalyst to accept N 2 lone-pair electrons. [8,9] Second, the potentials needed to proceed with the electrochemical NRR are usually similar to that required for the hydrogen evolution reaction (HER). [10,11] During the conversion from N 2 to NH 3 , the attendant HER competes for the consumption of electrons reducing the Faraday efficiency. Therefore, it is highly desirable but still remains a challenge to design an electrocatalytic system that could efficiently and selectively electroreduction of N 2 to NH 3 .The general electrocatalytic NRR process involves the adsorption of N 2 on active sites and the subsequent combination of protons (and electrons for the hydrogenation of the bound N 2 . [12,13] To achieve these multiple H-coupled electrontransfer steps, various kinds of heterogeneous electrocatalysts have been examined for NRR, such as transition metals, metal oxides, nitrides, sulfides, carbides, and borides. [14][15][16][17][18][19] A few heterogeneous transition metal based catalysts have been proven effective for increasing the N 2 adsorption and alleviating the reaction barriers. However, since general metal catalysts are inherently more inclined to adsorb H, most active sites and electrons are occupied and consumed by unwanted hydrogen atoms, leading to a domination of the competing HER over the NRR and the impediment of the NRR catalytic activity and selectivity. [20,21] To improve the NRR selectivity, various methods like limiting the accessibility of H and electrons, changing the chemical equilibrium of the HER, and designing catalysts to reduce the HER activity have been employed to suppress the HER. [20][21][22][23][24][25][26][27] Among them, studies focusing on the investigation of supports for a stronger adsorption of N 2 than H to inhibit the HER and improve the overall conversion of N 2 to NH 3The electrochemical nitrogen reduction reaction (NRR) has the potential to replace the Haber-Bosch process for ammonia synthesis under ambient conditions. However, the selectivity and yield of the NRR are impractical, owing to the preferential binding of the electrocatalyst to H and the consequential coverage of active sites. In this study, VO 2 , with N 2 strongly adsorbed over H atoms, is used as a support to provide a N 2 source to avoid the hydrogen evolution reaction. Mo, with a high NRR activity, is introduced as the active site to promote the NRR. Meanwhile, the electronic metal-su...

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Section: Introductionmentioning

confidence: 99%

Improving Electrocatalytic Nitrogen Reduction Selectivity and Yield by Suppressing Hydrogen Evolution Reaction via Electronic Metal–Support Interaction

Xie

Dai

Guo

et al. 2023

Advanced Energy Materials

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“…Notably, AOPs facilitate the complete oxidation of organic contaminants into harmless byproducts like water and carbon dioxide. 16,17 While research into AOPs, particularly those centered on photocatalysts, has made significant strides, most photocatalytic materials exhibit limited photoresponse spans and a constrained number of active sites for catalytic reactions. Moreover, they are prone to recombination of photogenerated electron-hole pairs, thereby impinging on their catalytic efficacy and rendering them suboptimal for practical applications.…”

Section: Introductionmentioning

confidence: 99%

“…The current catalysts for the degradation of organic pollution by CWAO include metal oxides, noble metal catalysts, and polymetallic oxides. 16,17,21,22 For instance, Estrella et al achieved nearly 100% dye removal of naproxen using the CNS-Ru catalyst at 130 1C and 20 bar in 1.5 h. 23 Burcu et al investigated the catalytic performance of biomimetic metal oxides in wet-aircatalyzed oxidation processes, achieving 98.3% degradation of a 100 mg L À1 acetaminophen solution via a 1 g L À1 biomimetic CuO catalyst at 180 1C and 10 bar. 24 Furthermore, Dai et al fabricated well-structured multilayered Cu 2 (OH) 3 NO 3 nanosheets using metal oxides, resulting in approximately 97% decolorization of Cu 2 (OH) 3 NO 3 /ZnO composites against methyl orange (MO) within 20 min at room temperature in the dark.…”

Section: Introductionmentioning

confidence: 99%

Plasma synthesis of oxygen vacancy-rich CuO/Cu₂(OH)₃NO₃ heterostructure nanosheets for boosting degradation performance

Yang,

Peng,

Zheng

et al. 2023

Phys. Chem. Chem. Phys.

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Improving Generation Performance of ¹O₂ by Atomic Doping for Efficient Catalytic Advanced Oxidation Processes

Qi,

Wang,

Zhang

et al. 2024

Adv Funct Materials

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Singlet oxygen (1O2) has attracted great attention owing to its superior comprehensive oxidizing performance and extensive application in dealing with ever‐growing environmental pollution. However, the efficient catalytic generation of 1O2 is very challenging due to the low catalytic activity of most catalysts and the generation of oxygen‐containing radicals in the catalytic reaction. Herein, C‐doped Co nanoparticles (CoNPs) supported on porous carbon (C─Co/C) as highly reactive and selective 1O2‐producing catalysts are demonstrated for efficient catalytic oxidation of recalcitrant organics via activation of peroxymonosulfate (PMS). The doped C 2p orbitals can accept Co 3d electrons, thereby weakening the Co─O bonding between Co and PMS or other oxygen‐containing intermediates such as *SO4, *OH, *OOH, and *O. The adsorption and cleavage energy of PMS on Co nanoparticle is reduced from 8.09 to 4.64 eV by C doping. The energy barrier of the *OOH to 1O2 step is also lowered significantly, thereby kinetically improving the activity for the generation of 1O2. The C─Co/C catalysts promotes the efficient and 100% selective generation of 1O2 with high modified kinetic model (K) values of 457.0 and 94.5 µmol s−1 g−1 for rhodamine (RhB) and 2,4‐dichlorophenol (2,4‐DCP), respectively.

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N, O-dual coordination regulation directs the design of active sites on nanoclusters for highly efficient catalytic water purification

Cited by 14 publications

References 56 publications

Improving Electrocatalytic Nitrogen Reduction Selectivity and Yield by Suppressing Hydrogen Evolution Reaction via Electronic Metal–Support Interaction

Improving Electrocatalytic Nitrogen Reduction Selectivity and Yield by Suppressing Hydrogen Evolution Reaction via Electronic Metal–Support Interaction

Plasma synthesis of oxygen vacancy-rich CuO/Cu₂(OH)₃NO₃ heterostructure nanosheets for boosting degradation performance

Improving Generation Performance of ¹O₂ by Atomic Doping for Efficient Catalytic Advanced Oxidation Processes

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N, O-dual coordination regulation directs the design of active sites on nanoclusters for highly efficient catalytic water purification

Cited by 14 publications

References 56 publications

Improving Electrocatalytic Nitrogen Reduction Selectivity and Yield by Suppressing Hydrogen Evolution Reaction via Electronic Metal–Support Interaction

Improving Electrocatalytic Nitrogen Reduction Selectivity and Yield by Suppressing Hydrogen Evolution Reaction via Electronic Metal–Support Interaction

Plasma synthesis of oxygen vacancy-rich CuO/Cu2(OH)3NO3 heterostructure nanosheets for boosting degradation performance

Improving Generation Performance of 1O2 by Atomic Doping for Efficient Catalytic Advanced Oxidation Processes

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Product

Resources

About

Plasma synthesis of oxygen vacancy-rich CuO/Cu₂(OH)₃NO₃ heterostructure nanosheets for boosting degradation performance

Improving Generation Performance of ¹O₂ by Atomic Doping for Efficient Catalytic Advanced Oxidation Processes