The critical role of electrochemically activated adsorbates in neutral OER

Zhang, Longsheng; Yuan, Haiyang; Wang, Liping; Zhang, Hui; Zang, Yijing; Tian, Yao; Wen, Yunzhou; Ni, Fenglou; Song, Hao; Wang, Haifeng; Zhang, Bo; Peng, Huisheng

doi:10.1007/s40843-020-1390-6

Cited by 21 publications

(13 citation statements)

References 32 publications

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“…Unfortunately, this technique has rarely been applied to study the reconstruction of electrocatalysts. [ 45 ] Due to its extremely high sensitivity, the LEIS requires ultra‐high vacuum conditions and the signal could be blocked by unexpected surface contaminations. Fourier‐transform infrared spectroscopy (FTIR) is conducted by achieving the transitions of vibrational and rotational energy levels from the ground state to the excited state under the continuous change of infrared light.…”

Section: Reconstruction Of Electrocatalystsmentioning

confidence: 99%

Surface Reconstruction of Water Splitting Electrocatalysts

Zeng

Zhao

Huang

et al. 2022

Advanced Energy Materials

155

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Gibbs free energy (ΔG) of water splitting reaction is 237.2 kJ mol −1 , corresponding to a theoretical voltage of 1.23 V. [3] However, the existence of electrochemical/concentration polarization and solution resistance can increase the actual voltage of water electrolysis to much beyond 1.23 V. Particularly, the OER involves a complicated four-electron transfer process, which results in a sluggish kinetics thus has long been the bottleneck. [4] Therefore, it is necessary to explore efficient and robust electrocatalysts to reduce the overpotential of water electrolysis and the extra electric energy consumption. Although noble electrocatalysts, such as Pt, RuO 2 and IrO 2 , are recognized as the most efficient electrocatalysts for water electrolysis, their high scarcity and instability severely impede large-scale applications. [5] Recently, considerable effort has been focused on nonnoble transition-metal materials as viable alternatives for water splitting. Understanding the intrinsic catalytic mechanism and real active sites of these catalysts will benefit the rational design and application of high-efficiency catalysts.With the development of in situ characterization technologies, more reports have revealed that the original electrocatalyst (so-called "pre-catalyst") surface sites would undergo dynamic reconstruction and transform into real reactive species. [6] This in situ reconstruction process could tune the electrocatalytic behaviors such as adsorption, activation, and desorption, thus improving the catalytic performance. [7] On this basis, many researchers utilized the pre-reconstruction of electrocatalysts to obtain a large number of active species for the catalytic reactions. [8] It has been found that the intrinsic properties of the pre-catalysts, such as composition, atomic arrangement, porosity, and crystallinity, would affect the reconstruction rate, reconstruction degree, and catalytic activity of the reconstructed species. [9] Moreover, the reaction conditions also affect the reconstruction process, such as electrochemical operation, applied potential, electrolyte concentration, and pH. [6a] Therefore, tuning the reconstruction process to generate abundant active sites with high intrinsic activity is an effective strategy to boost the catalytic performance of electrocatalysts.Although some influential review articles on the reconstruction of catalysts during water electrolysis have emerged, [10] most of them focus on the discovery and characterization of the reconstruction phenomenon, less on the regulation of the reconstruction process. In addition, reconstructed catalysts for Water electrolysis is regarded as an efficient and green method to produce hydrogen gas, a clean energy carrier that holds the key to solving global energy problems. So far, the efficiency and large-scale application of water electrolysis are restricted by the electrocatalytic activity of applied catalysts. Recently, the reconstruction phenomenon of electrocatalysts during a catalytic reaction has been discovered, which ...

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Section: Reconstruction Of Electrocatalystsmentioning

confidence: 99%

Surface Reconstruction of Water Splitting Electrocatalysts

Zeng

Zhao

Huang

et al. 2022

Advanced Energy Materials

155

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“…In CV, the morphological evolution was monitored by in situ TEM. [120][121][122] The in situ electrochemical transmission electron microscope support is shown in Figure 7. It consists of a disposable micro-three-electrode battery (electrochemical chip).…”

Section: In Situ Temmentioning

confidence: 99%

Progress in In Situ Research on Dynamic Surface Reconstruction of Electrocatalysts for Oxygen Evolution Reaction

Shen

Yin

Jin

et al. 2022

Adv Energy and Sustain Res

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Renewable energy and sustainable development have attracted considerable attention due to the rapid growth of energy consumption and environmental pollution. The further development of electrocatalytic water splitting can promote the development and application of next‐generation sustainable energy systems. However, the lack of an in‐depth understanding of the dynamic restructuring process occurring on the catalyst surface in the oxygen evolution reaction (OER) has limited the further development and improvement of OER‐related theories. Therefore, real‐time monitoring and analysis of the dynamic surface reconstruction process has a great significance for deeply understanding the intrinsic catalytic mechanism of OER. Herein, the latest progress on the in situ methods for characterizing the surface reconstruction of various transition metal‐based OER electrocatalysts in recent years is summarized. Many commonly methods used in situ characterization techniques have been reviewed to reveal the correlation between structure, surface reconstruction, and intrinsic activity.

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“…Unfortunately, these UOR catalysts still exhibit unsatisfactory activity due to the unfavorably strong absorption of the intermediate COO* on Ni 3+ sites [13] . It is reported that the adsorption energy of intermediates was closely related to its electronic structures [14–17] . Thus, regulating the electronic structures of Ni 3+ sites may construct catalytic sites with high UOR intrinsic activity.…”

Section: Figurementioning

confidence: 99%

Regulating the Local Charge Distribution of Ni Active Sites for the Urea Oxidation Reaction

et al. 2021

Self Cite

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In electrochemical energy storage and conversion systems, the anodic oxygen evolution reaction (OER) accounts for a large proportion of the energy consumption. The electrocatalytic urea oxidation reaction (UOR) is one of the promising alternatives to OER, owing to its low thermodynamic potential. However, owing to the sluggish UOR kinetics, its potential in practical use has not been unlocked. Herein, we developed a tungsten‐doped nickel catalyst (Ni‐WOx) with superior activity towards UOR. The Ni‐WOx catalyst exhibited record fast reaction kinetics (440 mA cm−2 at 1.6 V versus reversible hydrogen electrode) and a high turnover frequency of 0.11 s−1, which is 4.8 times higher than that without W dopants. In further experiments, we found that the W dopant regulated the local charge distribution of Ni atoms, leading to the formation of Ni3+ sites with superior activity and thus accelerating the interfacial catalytic reaction. Moreover, when we integrated Ni‐WOx into a CO2 flow electrolyzer, the cell voltage is reduced to 2.16 V accompanying with ≈98 % Faradaic efficiency towards carbon monoxide.

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The critical role of electrochemically activated adsorbates in neutral OER

Cited by 21 publications

References 32 publications

Surface Reconstruction of Water Splitting Electrocatalysts

Surface Reconstruction of Water Splitting Electrocatalysts

Progress in In Situ Research on Dynamic Surface Reconstruction of Electrocatalysts for Oxygen Evolution Reaction

Regulating the Local Charge Distribution of Ni Active Sites for the Urea Oxidation Reaction

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