Dynamic reconstructuring of CuS/SnO2-S for promoting CO2 electroreduction to formate

Dou, Tong; He, Jinqing; Diao, Shuteng; Wang, Yiping; Zhao, Xuhui; Zhang, Fazhi; Lei, Xiaodong

doi:10.1016/j.jechem.2023.03.016

Cited by 26 publications

(6 citation statements)

References 62 publications

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“…Such new surface speciation is bound to change the catalytic behaviour of CO 2 RR on the evolved SnO 2 . Figure 3a suggests the CO 2 RR mechanism toward HCOOH and CO on electrocatalysts, [3e,6a,14] where CO is produced following the reaction pathway of *COOH→*CO→CO, while HCOOH can be produced from two key intermediates, *COOH (*COOH+[H + + e − ]→*+HCOOH) and *OCHO (*OCHO+[H + + e − ]→*+HCOOH). First, the adsorption strengths of key CO 2 RR intermediates, *COOH and *OCHO, were analyzed on p‐SnO 2 and s‐SnO 2 .…”

Section: Resultsmentioning

confidence: 99%

Deciphering Structure‐Activity Relationship Towards CO₂ Electroreduction over SnO₂ by A Standard Research Paradigm

Guo,

Yu,

et al. 2024

Angewandte Chemie

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Authentic surface structures under reaction conditions determine the activity and selectivity of electrocatalysts, therefore, the knowledge of the structure−activity relationship can facilitate the design of efficient catalyst structures for specific reactivity requirements. However, understanding the relationship between a more realistic active surface and its performance is challenging due to the complicated interface microenvironment in electrocatalysis. Herein, we proposed a standard research paradigm to effectively decipher the structure−activity relationship in electrocatalysis, which is exemplified in the CO2 electroreduction over SnO2. The proposed practice has aided in discovering authentic/resting surface states (Sn layer) of SnO2 accountable for the electrochemical CO2 reduction reaction (CO2RR) performance under electrocatalytic conditions, which then is corroborated in the subsequent CO2RR experiments over SnO2 with different morphologies (nanorods, nanoparticles, and nanosheets) in combination with in−situ characterizations. This proposed methodology is further extended to the SnO electrocatalysts, providing helpful insights into catalytic structures. It is believed that our proposed standard research paradigm is also applicable to other electrocatalytic systems, in the meantime, decreases the discrepancy between theory and experiments, and accelerates the design of catalyst structures that achieve sustainable performance for energy conversion.

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Section: Resultsmentioning

confidence: 99%

Deciphering Structure‐Activity Relationship Towards CO₂ Electroreduction over SnO₂ by A Standard Research Paradigm

Guo,

Yu,

et al. 2024

Angewandte Chemie

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“…Figure a exhibits the TEM image of CuS/ZnS HNs with a length of 80 nm and thickness of 8 nm. CuS/ZnS HNs were further characterized by high-resolution TEM (HRTEM), selected-area electron diffraction (SAED), EDS, and XRD to investigate their structure and composition information. , In Figure b, the lattice spacings of 0.32 and 0.28 nm appearing in areas I and II were ascribed to the (0010) plane and (005) plane of ZnS and CuS. The EDS elemental mapping of CuS/ZnS HNs (Figure d,e) indicates three elements including Cu, Zn, and S. The line-scan profile result demonstrates the obvious hollow heterostructure (Figure f).…”

Section: Resultsmentioning

confidence: 99%

Plasmon-Stimulated Colorimetry Biosensor Array for the Identification of Multiple Metabolites

Tian,

Cao,

Cheng

et al. 2024

ACS Appl. Mater. Interfaces

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Rationally designing highly catalytic and stable nanozymes for metabolite monitoring is of great importance because of their huge potential in early disease diagnosis. Herein, a novel nanozyme based on hierarchically structured CuS/ZnS with a highly efficient peroxidase (POD)-mimic capability was developed and synthesized for multiple metabolite determination and recognition via the plasmon-stimulated biosensor array strategy. The designed nanozyme can simultaneously harvest plasmon triggered hot electron−hole pairs and generate photothermal properties, leading to a sharply boosted POD-mimic capability under 808 nm laser irradiation. Interestingly, because of the interaction diversity of the metabolite with POD-like nanomaterials, the unique inhibitory effect of metabolites on the PODmimic activity could be the signal response as the differentiation. Thus, utilizing TMB as a typical chromogenic substrate in the addition of H 2 O 2 , the designed colorimetric biosensor array can produce diverse fingerprints for the three vital metabolisms (cysteine (Cys), ascorbic acid (AA), and glutathione (GSH)), which can be precisely identified by principal component analysis (PCA). Notably, a distinct fingerprint of a single metabolite with different levels and metabolite mixtures is also achieved with a detection limit of 1 μM. Most importantly, cell lysis could be effectively discriminated by the biosensor assay, implying its great potential in clinical diagnosis.

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“…Both in situ ATR‐FTIR and in situ Raman were detected from the open circuit potential (OCP) to −1.2 V in CO 2 ‐saturated 0.5 m KHCO 3 electrolyte. In Figure 4c, the peak at 2300–2400 cm −1 belongs to CO 2 adsorption, [ 48–49 ] and the obvious peaks at 1635 and 3000–3600 cm −1 are assigned to the vibration of δ(H‐O‐H) and δ(O‐H) of water molecules. [ 31 ] The characteristic peaks at 1275 and 1440 cm −1 are attributed to the O‐C‐O vibration of the dioxygen bridge in * OCHO, [ 50 ] which gradually strengthens with the increase of applied potential, indicating the continuous production of formate.…”

Section: Resultsmentioning

confidence: 99%

Metal‐Organic Framework Derived Bi‐O‐Sn/C Nanostructure: Tailoring the Adsorption Site of Dominant Intermediate for Highly Efficient CO₂ Electroreduction to Formate

Wang,

Shao,

Zhang

et al. 2023

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Electrochemical CO2 reduction into high‐value‐added formic acid/formate is an attractive strategy to mitigate global warming and achieve energy sustainability. However, the adsorption energy of most catalysts for the key intermediate *OCHO is usually weak, and how to rationally optimize the adsorption of *OCHO is challenging. Here, an effective Bi‐Sn bimetallic electrocatalyst (Bi1‐O‐Sn1@C) where a Bi‐O‐Sn bridge‐type nanostructure is constructed with O as an electron bridge is reported. The electronic structure of Sn is precisely tuned by electron transfer from Bi to Sn through O bridge, resulting in the optimal adsorption energy of intermediate *OCHO on the surface of Sn and the enhanced activity for formate production. Thus, the Bi1‐O‐Sn1@C exhibits an excellent Faradaic efficiency (FE) of 97.7% at −1.1 V (vs RHE) for CO2 reduction to formate (HCOO−) and a high current density of 310 mA cm−2 at −1.5 V, which is one of the best results catalyzed by Bi‐ and Sn‐based catalysts reported previously. Impressively, the FE exceeds 93% at a wide potential range from −0.9 to −1.4 V. In‐situ ATR–FTIR, in‐situ Raman, and DFT calculations confirm the unique role of the bridge‐type structure of Bi‐O‐Sn in highly efficient electrocatalytic reduction of CO2 into formate.

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Dynamic reconstructuring of CuS/SnO2-S for promoting CO2 electroreduction to formate

Cited by 26 publications

References 62 publications

Deciphering Structure‐Activity Relationship Towards CO₂ Electroreduction over SnO₂ by A Standard Research Paradigm

Deciphering Structure‐Activity Relationship Towards CO₂ Electroreduction over SnO₂ by A Standard Research Paradigm

Plasmon-Stimulated Colorimetry Biosensor Array for the Identification of Multiple Metabolites

Metal‐Organic Framework Derived Bi‐O‐Sn/C Nanostructure: Tailoring the Adsorption Site of Dominant Intermediate for Highly Efficient CO₂ Electroreduction to Formate

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Dynamic reconstructuring of CuS/SnO2-S for promoting CO2 electroreduction to formate

Cited by 26 publications

References 62 publications

Deciphering Structure‐Activity Relationship Towards CO2 Electroreduction over SnO2 by A Standard Research Paradigm

Deciphering Structure‐Activity Relationship Towards CO2 Electroreduction over SnO2 by A Standard Research Paradigm

Plasmon-Stimulated Colorimetry Biosensor Array for the Identification of Multiple Metabolites

Metal‐Organic Framework Derived Bi‐O‐Sn/C Nanostructure: Tailoring the Adsorption Site of Dominant Intermediate for Highly Efficient CO2 Electroreduction to Formate

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Deciphering Structure‐Activity Relationship Towards CO₂ Electroreduction over SnO₂ by A Standard Research Paradigm

Deciphering Structure‐Activity Relationship Towards CO₂ Electroreduction over SnO₂ by A Standard Research Paradigm

Metal‐Organic Framework Derived Bi‐O‐Sn/C Nanostructure: Tailoring the Adsorption Site of Dominant Intermediate for Highly Efficient CO₂ Electroreduction to Formate