Ultrathin polycrystalline Co3O4 nanosheets with enriched oxygen vacancies for efficient electrochemical oxygen evolution and 5-hydroxymethylfurfural oxidation

Zhong, Renbin; Wang, Qi; Du, Lei; Pu, Yayun; Ye, Siyu; Gu, Meng; Zhang, Z. Conrad; Huang, Limin

doi:10.1016/j.apsusc.2022.152553

Cited by 35 publications

(38 citation statements)

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“…In addition to monomial transition metal oxides, 86 high‐entropy oxides (HEOs) have also stimulated research enthusiasm. Wang's group synthesized oxygen‐enriched vacancies of P‐HEOs ((FeCrCoNiCu) 3 O 4 ) nanosheets by low‐temperature plasma method, showing higher specific surface area and intrinsic activity than C‐HEOs prepared by high‐temperature calcination method, which greatly improved the performance of HMFOR 18 .…”

Section: Design Strategies For Electrocatalystsmentioning

confidence: 99%

“…[80][81][82] Therefore, Mu's team proposed for the first time that the adsorption energy of HMF on the catalyst surface is a potential activity descriptor for the HMFOR and further clarified the rationality of the adsorption energy of HMF as a descriptor. 79 In addition to monomial transition metal oxides, 86 highentropy oxides (HEOs) have also stimulated research enthusiasm. Wang's group synthesized oxygen-enriched vacancies of P-HEOs ((FeCrCoNiCu) 3 O 4 ) nanosheets by low-temperature plasma method, showing higher specific surface area and intrinsic activity than C-HEOs prepared by high-temperature calcination method, which greatly improved the performance of HMFOR.…”

Section: Defectsmentioning

confidence: 99%

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Electrocatalytic oxidation of 5‐hydroxymethylfurfural for sustainable 2,5‐furandicarboxylic acid production—From mechanism to catalysts design

Jiang

Liu

et al. 2023

SusMat

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Catalytic conversion of biomass-based platform chemicals is one of the significant approaches to utilize renewable biomass resources. 2,5-Furandicarboxylic acid (FDCA), obtained by an electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF), has attracted extensive attention due to the potential of replacing terephthalic acid to synthesize high-performance polymeric materials for commercialization. In the present work, the pHdependent reaction pathways and factors influencing the degree of functional group oxidation are first discussed. Then the reaction mechanism of HMF oxidation is further elucidated using the representative examples. In addition, the emerging catalyst design strategies (defects, interface engineering) used in HMF oxidation are generalized, and structure-activity relationships between the abovementioned strategies and catalysts performance are analyzed. Furthermore, cathode pairing reactions, such as hydrogen evolution reaction, CO 2 reduction reaction (CO 2 RR), oxygen reduction reaction, and thermodynamically favorable organic reactions to lower the cell voltage of the electrolysis system, are discussed. Finally, the challenges and prospects of the electrochemical oxidation of HMF for FDCA are presented, focusing on deeply investigated reaction mechanism, coupling reaction, reactor design, and downstream product separation/purification.

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Section: Design Strategies For Electrocatalystsmentioning

confidence: 99%

Section: Defectsmentioning

confidence: 99%

Electrocatalytic oxidation of 5‐hydroxymethylfurfural for sustainable 2,5‐furandicarboxylic acid production—From mechanism to catalysts design

Jiang

Liu

et al. 2023

SusMat

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“…The CoO x H y nanosheets were synthesized by a simple template-assisted solvothermal method. 10 Concretely, 0.5 g P123 (EO 20 PO 70 EO 20 , M w = 5800 g mol −1 ) was dissolved in a mixed solvent composed of 7.5 g ethanol, 2.5 g H 2 O, and 30 mL ethylene glycol by sonication to form the template solution. 1.25 mmol of cobalt acetate tetrahydrate (Co (OOCCH 3 ) 2 •4H 2 O) and 1.25 mmol of hexamethylenetetramine (HMTA) were then added in the P123 solution under vigorous stirring for 30 min.…”

Section: Preparation Of Catalystsmentioning

confidence: 99%

“…7,8 Our previous work reported a topotactic conversion of two-dimensional (2D) cobalt oxide hydrate (CoO x H y ) to surfactant-free and polycrystalline Co 3 O 4 nanosheets with enriched oxygen vacancies at grain boundaries via rapid calcination at 300 °C for 5 min to improve the HMFOR performance. 10 The temperature of 300 °C was chosen to remove the surfactant to expose the catalyst surface and simultaneously maintain the ultrathin 2D structure. Nevertheless, heat treatment still caused the loss of active surfaces with increased crystallinity.…”

Section: Introductionmentioning

confidence: 99%

Room-temperature fabrication of defective CoO_xH_y nanosheets with abundant oxygen vacancies and high porosity as efficient 5-hydroxymethylfurfural oxidation electrocatalysts

Zhong

Wang

et al. 2023

Green Chem.

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“…[45][46][47] Compared with other metal oxides, perovskite oxides with good flexibility of crystal structures can allow their metal cations to exist in abnormal or mixed valence states, thus resulting in enriched oxygen vacancies in their structures. [48][49][50][51] We further carried out EPR spectroscopy to study the amount of oxygen vacancies through detecting unpaired electrons in these perovskites. As shown in Figure 3c, the LaCrO 3 , LaMnO 3 , LaFeO 3 , and LaCoO 3 all show obvious EPR signals at g = 2.003.…”

Section: Resultsmentioning

confidence: 99%

Perovskites with Enriched Oxygen Vacancies as a Family of Electrocatalysts for Efficient Nitrate Reduction to Ammonia

Zheng

Zhang

Wang

et al. 2022

Small

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Haber-Bosch approach, which involves high pressures (10−30 MPa) and temperatures (400−500 °C), large consumption of coal and natural gas to produce hydrogen, leading to excessive emission of carbon dioxide and serious environmental issues. [4][5][6][7] In this regard, developing an efficient, sustainable approach for NH 3 synthesis is urgently desired. Recently, electrochemical nitrogen (N 2 ) reduction reaction (NRR) toward NH 3 synthesis has attracted enormous attention as a feasible approach under ambient conditions. Unfortunately, the low solubility of N 2 in aqueous electrolytes and high fracture energy of the triple bond of N 2 (941 kJ mol −1 ) significantly hinder the improvement of catalytic activity for NRR. [8][9][10] Besides, the energetically favorable hydrogen evolution reaction (HER) as a competitive reaction of NRR would decrease the Faradaic efficiency of N 2 electroreduction to NH 3 , which severely limits the practical applications of NRR toward NH 3 synthesis. [11][12][13][14][15] Alternatively, electrochemical nitrate (NO 3 − ) reduction to NH 3 (NRA) can provide a promising approach for efficient NH 3 synthesis, due to the smaller dissociation energy of NO bond (204 kJ mol −1 ), the higher solubility of NO 3 − in aqueous electrolytes and endowing faster reaction kinetics. [16][17][18][19] Meanwhile, the NRA catalysis can utilize NO 3 − from abundant wastewater or groundwater, offering an avenue to convert NO 3 − into value-added products to restore the imbalance of global nitrogen cycle. Such approach can address the environmental issues caused by the widely existed NO 3 − pollutants in nature that would become a safety hazard for human health, but also offer efficient utilization of NH 3 -related energy sources simultaneously. [20,21] Nevertheless, the NRA electrolysis suffers from large thermodynamic barriers due to its complex eight-electron reaction process and the competitive HER. [22] Tailoring the environments on the catalyst surface to modulate the adsorption of NRA intermediates and suppress the HER rate will hinder the formation of byproducts and boost the selective reduction of NO 3 − to NH 3 . Thus, designing and constructing efficient NRA electrocatalysts with optimized adsorption properties of NO 3 − and reaction intermediates on the catalyst surface are urgently desired.Electrochemical nitrate reduction to ammonia (NRA) provides an efficient, sustainable approach to convert the nitrate pollutants into value-added products, which is regarded as a promising alternative to the industrial Haber-Bosch process. Recent studies have shown that oxygen vacancies of oxide catalysts can adjust the adsorption energies of intermediates and affect their catalytic performance. Compared with other metal oxides, perovskite oxides can allow their metal cations to exist in abnormal or mixed valence states, thereby resulting in enriched oxygen vacancies in their crystal structures. Here, the catalytic activities of perovskite oxides toward NRA catalysis with respect to the amount of oxygen vacanci...

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Ultrathin polycrystalline Co3O4 nanosheets with enriched oxygen vacancies for efficient electrochemical oxygen evolution and 5-hydroxymethylfurfural oxidation

Cited by 35 publications

References 35 publications

Electrocatalytic oxidation of 5‐hydroxymethylfurfural for sustainable 2,5‐furandicarboxylic acid production—From mechanism to catalysts design

Electrocatalytic oxidation of 5‐hydroxymethylfurfural for sustainable 2,5‐furandicarboxylic acid production—From mechanism to catalysts design

Room-temperature fabrication of defective CoO_xH_y nanosheets with abundant oxygen vacancies and high porosity as efficient 5-hydroxymethylfurfural oxidation electrocatalysts

Perovskites with Enriched Oxygen Vacancies as a Family of Electrocatalysts for Efficient Nitrate Reduction to Ammonia

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Ultrathin polycrystalline Co3O4 nanosheets with enriched oxygen vacancies for efficient electrochemical oxygen evolution and 5-hydroxymethylfurfural oxidation

Cited by 35 publications

References 35 publications

Electrocatalytic oxidation of 5‐hydroxymethylfurfural for sustainable 2,5‐furandicarboxylic acid production—From mechanism to catalysts design

Electrocatalytic oxidation of 5‐hydroxymethylfurfural for sustainable 2,5‐furandicarboxylic acid production—From mechanism to catalysts design

Room-temperature fabrication of defective CoOxHy nanosheets with abundant oxygen vacancies and high porosity as efficient 5-hydroxymethylfurfural oxidation electrocatalysts

Perovskites with Enriched Oxygen Vacancies as a Family of Electrocatalysts for Efficient Nitrate Reduction to Ammonia

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Room-temperature fabrication of defective CoO_xH_y nanosheets with abundant oxygen vacancies and high porosity as efficient 5-hydroxymethylfurfural oxidation electrocatalysts