A Glass‐Ceramic with Accelerated Surface Reconstruction toward the Efficient Oxygen Evolution Reaction

Li, Shanlin; Li, Zichuang; Ma, Ruguang; Gao, Chunlang; Liu, Linlin; Hu, Lanping; Zhu, Jinlin; Sun, Tongming; Tang, Yanfeng; Liu, Danmin; Wang, Jiacheng

doi:10.1002/anie.202014210

Cited by 189 publications

(128 citation statements)

References 58 publications

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“…29a, b ), suggesting a possible catalyst activation process. This might be a result of catalyst surface reconstruction, which has been identified in many electrocatalysts (especially for OER) 39 , 47 , 48 and photocatalysts 49 , 50 . For better understanding of the reconstruction of the catalyst, a carbon cloth-supported CoNi 0.25 P catalyst was prepared (Supplementary Fig.…”

Section: Resultsmentioning

confidence: 99%

“…In addition, the lower activity of CoNi 0.25 (OH) 2 /NF-derived oxy(hydroxide) and oxide compared with its phosphide (CoNi 0.25 P/NF) indicates the important role of phosphorization in improving the activity and selectivity for cutting C–C in EG to formate (Supplementary Figs.17 and 18a). This may be attributed to that the phosphorization can accelerate the reconstruction of materials toward active catalyst 39 , and lower the charge transfer resistance (Supplementary Fig. 18b ).…”

Section: Resultsmentioning

confidence: 99%

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Electrocatalytic upcycling of polyethylene terephthalate to commodity chemicals and H2 fuel

et al. 2021

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Plastic wastes represent a largely untapped resource for manufacturing chemicals and fuels, particularly considering their environmental and biological threats. Here we report electrocatalytic upcycling of polyethylene terephthalate (PET) plastic to valuable commodity chemicals (potassium diformate and terephthalic acid) and H2 fuel. Preliminary techno-economic analysis suggests the profitability of this process when the ethylene glycol (EG) component of PET is selectively electrooxidized to formate (>80% selectivity) at high current density (>100 mA cm−2). A nickel-modified cobalt phosphide (CoNi0.25P) electrocatalyst is developed to achieve a current density of 500 mA cm−2 at 1.8 V in a membrane-electrode assembly reactor with >80% of Faradaic efficiency and selectivity to formate. Detailed characterizations reveal the in-situ evolution of CoNi0.25P catalyst into a low-crystalline metal oxy(hydroxide) as an active state during EG oxidation, which might be responsible for its advantageous performances. This work demonstrates a sustainable way to implement waste PET upcycling to value-added products.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Electrocatalytic upcycling of polyethylene terephthalate to commodity chemicals and H2 fuel

et al. 2021

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“…Therefore, the dynamic surface chemistry is controlled by both electrolyte composition and surface terminations of catalysts, where it triggers favorable oxygen‐containing intermediate steps. [ 79 ] Another rationality of the anion effect can be a lower local pH, compared with the situation without buffer or additives in the electrolyte, due to the competitivity of exotic anions with hydroxide anions.…”

Section: Correlation Between Dynamic Surface Chemistry and Reaction/servicing Conditionsmentioning

confidence: 99%

“…Such a potential‐dependent phase transformation and surface reconstruction has been revealed by in situ Raman investigations in several catalysts. [ 1,15b,79 ] As a result, on basis of these real‐time changes in composition of the OER catalysts and the nature of the catalytic site, most metal X‐ides can be referred to one of the three broad categories (Figure 8c). The first one is X‐ides themselves, where there are largely unchanged in surface structure even under rather rigorous OER conditions.…”

Section: In Situ Experimental Tracking Of Dynamic Surfacesmentioning

confidence: 99%

Dynamic Surface Chemistry of Catalysts in Oxygen Evolution Reaction

Kou

Zhang

et al. 2021

Small Science

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Electrocatalytic oxygen evolution reaction (OER) is a crucial anode reaction where electrocatalysts are the key elements and their dynamic surface chemistry runs throughout the entire process. Herein, we examine the latest advances and challenges in understanding of the dynamic surface chemistry of OER electrocatalysts. There are electrochemical origin and driving force for the dynamic surface nature, where several processes can take place either concurrently or sequentially, including reconstruction (i.e., phase formation/transformation, morphological change, and compositional change), vacancy generation and filling/refilling, and the intermediate adsorption-desorption process on catalytic surface. These dynamic surface processes of OER catalysts are impacted by not only the reaction and service conditions, including the (local) pH and its gradient distribution, applied potential, types and concentration of exotic ions and external fields on top of the nature of catalysts/precatalysts, but also their interactions. Due to the local, time-dependent and instant nature, there are considerable challenges in tracing, modelling and understanding of the complete dynamic surface chemistry of catalysts in OER, by means of ex situ, in situ and operando experimental investigations. Therefore, computational studies and dynamic simulations help provide key insights in future pursuits, where there is critical need for a multiscale computational modelling approach encompassing all these aspects.

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“…Recently, nonmetallic anionic groups, such as phosphate (PO 4 3− ), selenate (SeO 4 2− ), and sulfate (SO 4 2− ), have emerged as alternatives to boost water oxidation ability. [16][17][18] These nonmetallic groups could optimize the electronic structure of active sites, regulate the adsorption of intermediates to reduce OER overpotential, and promote the surface carrier transfer. Particularly, the SO 4 2− group can break the adsorption-energy scaling relation between OH* and OOH* (reaction intermediates) and decrease the OER overpotential.…”

mentioning

confidence: 99%

Incorporation of Sulfate Anions and Sulfur Vacancies in ZnIn₂S₄ Photoanode for Enhanced Photoelectrochemical Water Splitting

Gao

Meng

et al. 2021

Advanced Energy Materials

105

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friendly properties. [6] However, due to its severe bulk carrier recombination, unfavorable carrier transportation, and sluggish surface OER dynamics, the PEC performance of bare ZnIn 2 S 4 photoanode is still not satisfactory.Various strategies have been developed to enhance the PEC performance of ZnIn 2 S 4 , such as morphology engineering, constructing heterojunctions, and coating surface co-catalysts, etc. [7][8][9] Among them, decorating surface cocatalysts has been considered as an effective strategy to promote surface water oxidation kinetics of pristine ZnIn 2 S 4 . However, the integration of water-oxidation cocatalysts with PEC photoanodes has been limited to metal-based materials, such Co-Pi, FeCoO x , and FeOOH. [10][11][12][13][14][15] The cocatalysts containing metallic ions tend to be toxic and expensive, which could limit their further applications. In addition, these cocatalysts may cause light absorption attenuation and increased charge recombination due to the large thickness/dimension of cocatalysts and additional interface defects between cocatalysts and photo anodes. Recently, nonmetallic anionic groups, such as phosphate (PO 4 3− ), selenate (SeO 4 2− ), and sulfate (SO 4 2− ), have emerged as alternatives to boost water oxidation ability. [16][17][18] These nonmetallic groups could optimize the electronic structure of active sites, regulate the adsorption of intermediates to reduce OER overpotential, and promote the surface carrier transfer. Particularly, the SO 4 2− group can break the adsorption-energy scaling relation between OH* and OOH* (reaction intermediates) and decrease the OER overpotential. [17] Accordingly, engineering ZnIn 2 S 4 with SO 4 2− groups is a promising strategy to improve its surface reaction kinetics. However, the introduction of nonmetallic anionic groups usually relies on a direct mixing method or external addition, which leads to weak chemical interaction and thus decreases the effectiveness and durability of the resultant materials. [17] In contrast, in situ introducing SO 4 2− anionic groups into ZnIn 2 S 4 to induce strong bonding between anions and metal atoms is expected to remarkably facilitate solar water oxidation.As a kind of intrinsic defect for metal sulfide, sulfur vacancies (S v ) have the ability to adjust the electronic structure of metal sulfide, leading to optimization of the adsorption free energy and also improvement of the conductivity. [19,20] S v can be divided into bulk S v and surface S v according to their spatial Severe charge recombination and slow surface water oxidation kinetics seriously limit the practical application of ZnIn 2 S 4 photoanodes for photo electrochemical water splitting. Herein, an in situ strategy to introduce sulfate (SO 4 2− ) anions and controlled bulk sulfur vacancies (S v ) into a ZnIn 2 S 4 photoanode is developed, and its PEC performance is remarkably enhanced, achieving a photocurrent density of 3.52 mA cm −2 at 1.23 V versus reversible hydrogen electrode (V RHE ) and negatively shifted onset potential of 0....

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A Glass‐Ceramic with Accelerated Surface Reconstruction toward the Efficient Oxygen Evolution Reaction

Cited by 189 publications

References 58 publications

Electrocatalytic upcycling of polyethylene terephthalate to commodity chemicals and H2 fuel

Electrocatalytic upcycling of polyethylene terephthalate to commodity chemicals and H2 fuel

Dynamic Surface Chemistry of Catalysts in Oxygen Evolution Reaction

Incorporation of Sulfate Anions and Sulfur Vacancies in ZnIn₂S₄ Photoanode for Enhanced Photoelectrochemical Water Splitting

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A Glass‐Ceramic with Accelerated Surface Reconstruction toward the Efficient Oxygen Evolution Reaction

Cited by 189 publications

References 58 publications

Electrocatalytic upcycling of polyethylene terephthalate to commodity chemicals and H2 fuel

Electrocatalytic upcycling of polyethylene terephthalate to commodity chemicals and H2 fuel

Dynamic Surface Chemistry of Catalysts in Oxygen Evolution Reaction

Incorporation of Sulfate Anions and Sulfur Vacancies in ZnIn2S4 Photoanode for Enhanced Photoelectrochemical Water Splitting

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Product

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Incorporation of Sulfate Anions and Sulfur Vacancies in ZnIn₂S₄ Photoanode for Enhanced Photoelectrochemical Water Splitting