<i>In Situ</i> Electrocatalytic Infrared Spectroscopy for Dynamic Reactions

Liu, Hengjie; Qi, Zeming; Li, Song

doi:10.1021/acs.jpcc.1c07689

Cited by 39 publications

(35 citation statements)

References 127 publications

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“…An experimental study using advanced operando synchrotron radiation−Fourier transform infrared spectroscopy (SR-FTIR) was further conducted to justify the urea formation mechanism; 37 the experimental setup and cell are displayed in Figure S28. Figure 5g presents the infrared signals collected from 800 to 1800 cm −1 when the operando electrocatalysis test was performed on V O -InOOH during the negative scan from −0.3 to −1.0 V versus RHE.…”

Section: −1mentioning

confidence: 99%

A Defect Engineered Electrocatalyst that Promotes High-Efficiency Urea Synthesis under Ambient Conditions

et al. 2022

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Synthesizing urea from nitrate and carbon dioxide through an electrocatalysis approach under ambient conditions is extraordinarily sustainable. However, this approach still lacks electrocatalysts developed with high catalytic efficiencies, which is a key challenge. Here, we report the high-efficiency electrocatalytic synthesis of urea using indium oxyhydroxide with oxygen vacancy defects, which enables selective C–N coupling toward standout electrocatalytic urea synthesis activity. Analysis by operando synchrotron radiation–Fourier transform infrared spectroscopy showcases that *CO2NH2 protonation is the potential-determining step for the overall urea formation process. As such, defect engineering is employed to lower the energy barrier for the protonation of the *CO2NH2 intermediate to accelerate urea synthesis. Consequently, the defect-engineered catalyst delivers a high Faradaic efficiency of 51.0%. In conjunction with an in-depth study on the catalytic mechanism, this design strategy may facilitate the exploration of advanced catalysts for electrochemical urea synthesis and other sustainable applications.

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Section: −1mentioning

confidence: 99%

A Defect Engineered Electrocatalyst that Promotes High-Efficiency Urea Synthesis under Ambient Conditions

et al. 2022

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“…Researchers have developed effective strategies to endow these materials with active sites for N 2 RR, NO 3 RR, and C–N coupling. However, in-depth fundamental understanding of nitrogen conversion pathways still needs further exploration, which requires the combination of theoretical analyses (DFT or molecular dynamics simulations) with experimental validation (in situ Raman or operando FTIR) . The overall efficiency also needs to be further improved.…”

Section: Conclusion Challenges and Outlookmentioning

confidence: 99%

Emerging p-Block-Element-Based Electrocatalysts for Sustainable Nitrogen Conversion

Liu

Lee

et al. 2022

ACS Nano

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Artificial nitrogen conversion reactions, such as the production of ammonia via dinitrogen or nitrate reduction and the synthesis of organonitrogen compounds via C−N coupling, play a pivotal role in the modern life. As alternatives to the traditional industrial processes that are energy-and carbon-emission-intensive, electrocatalytic nitrogen conversion reactions under mild conditions have attracted significant research interests. However, the electrosynthesis process still suffers from low product yield and Faradaic efficiency, which highlight the importance of developing efficient catalysts. In contrast to the transition-metal-based catalysts that have been widely studied, the p-block-element-based catalysts have recently shown promising performance because of their intriguing physiochemical properties and intrinsically poor hydrogen adsorption ability. In this Perspective, we summarize the latest breakthroughs in the development of p-block-elementbased electrocatalysts toward nitrogen conversion applications, including ammonia electrosynthesis from N 2 reduction and nitrate reduction and urea electrosynthesis using nitrogen-containing feedstocks and carbon dioxide. The catalyst design strategies and the underlying reaction mechanisms are discussed. Finally, major challenges and opportunities in future research directions are also proposed.

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“…In situ IR spectroscopy was extensively used to reveal the CO 2 RR mechanisms by detecting the chemisorbed species on the electrode surface [163]. Then, the adsorbed species with unique vibrational modes such as *CO, adsorbed CO 3 2− , and *CO dimers can be analyzed in real time during the CO 2 RR.…”

Section: In Situ Characterization Techniquesmentioning

confidence: 99%

Rational Manipulation of Intermediates on Copper for CO2 Electroreduction Toward Multicarbon Products

Han

Gao

et al. 2022

Trans. Tianjin Univ.

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Excess greenhouse gas emissions, primarily carbon dioxide (CO2), have caused major environmental concerns worldwide. The electroreduction of CO2 into valuable chemicals using renewable energy is an ecofriendly approach to achieve carbon neutrality. In this regard, copper (Cu) has attracted considerable attention as the only known metallic catalyst available for converting CO2 to high-value multicarbon (C2+) products. The production of C2+ involves complicated C–C coupling steps and thus imposes high demands on intermediate regulation. In this review, we discuss multiple strategies for modulating intermediates to facilitate C2+ formation on Cu-based catalysts. Furthermore, several sophisticated in situ characterization techniques are outlined for elucidating the mechanism of C–C coupling. Lastly, the challenges and future directions of CO2 electroreduction to C2+ are envisioned.

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In Situ Electrocatalytic Infrared Spectroscopy for Dynamic Reactions

Cited by 39 publications

References 127 publications

A Defect Engineered Electrocatalyst that Promotes High-Efficiency Urea Synthesis under Ambient Conditions

A Defect Engineered Electrocatalyst that Promotes High-Efficiency Urea Synthesis under Ambient Conditions

Emerging p-Block-Element-Based Electrocatalysts for Sustainable Nitrogen Conversion

Rational Manipulation of Intermediates on Copper for CO2 Electroreduction Toward Multicarbon Products

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