In situ Raman spectroscopy reveals the structure and dissociation of interfacial water

Wang, Yaohui; Zheng, Shu Guo; Yang, Weimin; Zhou, Ru-Yu; He, Quanfeng; Radjenovic, Petar M.; Dong, Jin‐Chao; Li, Shunning; Zheng, Jiaxin; Yang, Zhilin; Attard, Gary Anthony; Pan, Feng; Tian, Zhong‐Qun; Li, Jianfeng

doi:10.1038/s41586-021-04068-z

Cited by 434 publications

(359 citation statements)

References 34 publications

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“…A sharp band at 1006 cm -1 can be assigned to C-O stretching of adsorbed ethoxy intermediate (10). A relatively small band at 931 cm -1 can be assigned to Cl-O stretching of perchlorate in the electrolyte solution (28), and another sharp band located at 770 cm -1 can be assigned to the -CH3 rocking vibration of ethoxy (22). It is well established that Raman bands around 570-630 cm -1 can be assigned to the surface adsorbed oxygen species on Cu (29,30), so it's not unexpected that the band located at 607 cm -1 tends to diminish as potential becomes more negative due to the reduction of surface oxygen.…”

Section: Resultsmentioning

confidence: 99%

Unraveling the Electrocatalytic Reduction Mechanism of Enols on Copper in Aqueous Media

Cui

Dong

Cho

et al. 2022

Preprint

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A mechanism is proposed for the direct electrochemical deoxygenation of aldehydes to alkenes and alkanes which has implications in refining biomass-derived fuels for use as transportation fuel, as a potential green synthesis strategy for terminal olefins in aqueous, ambient conditions, and in understanding the reaction pathway for CO2 to C2 and C3 products. Here we report the electrochemical conversion of vinyl alcohol and acetaldehyde on polycrystalline Cu to ethanol, ethylene and ethane; and propenol and propionaldehyde to propanol, propene and propane. Sensitive detection was achieved using a rotating disk electrode coupled with gas chromatography-mass spectrometry (RDE-GC-MS). In situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS), and in situ Raman spectroscopy confirmed the adsorption of the vinyl alcohol. Calculations using canonical and grand-canonical density functional theory (DFT and GC-DFT), along with experimental findings suggest that the rate-determining step (RDS) for ethylene and ethane formation is an electron transfer step to the adsorbed vinyl alcohol. Finally, we extend our conclusions to enols resulting from higher-order soluble aldehyde and ketone.

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Section: Resultsmentioning

confidence: 99%

Unraveling the Electrocatalytic Reduction Mechanism of Enols on Copper in Aqueous Media

Cui

Dong

Cho

et al. 2022

Preprint

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“…In 2021, Li group combined electrochemical method and Raman spectroscopy to study interfacial water on atomically flat Pd single-crystal surfaces with the help of computational techniques from the Pan group. [38] The direct spectroscopic evidences proved that interfacial water consists of hydrogen-bonded and hydrated Na + ion water (Figure 6a). Besides, they found that the ordered Na•H 2 O structure can strongly strengthen the Pd-H bonding interaction, which boosts HER activity at the interfacial level (Figure 6b).…”

Section: Monitoring Of Active Intermediates Via Spectroscopic Techniquesmentioning

confidence: 96%

“…[37] According to their results, H 2 O molecule is trend to form an icelike structure by strong hydrogen bonding with the surrounding water molecules at high potential (E>0.8 V), while does not interact with the adsorbed hydrogen at low potentials (E<0.4 V), indicating that the Pt‐H ads surface is hydrophobic. In 2021, Li group combined electrochemical method and Raman spectroscopy to study interfacial water on atomically flat Pd single‐crystal surfaces with the help of computational techniques from the Pan group [38] . The direct spectroscopic evidences proved that interfacial water consists of hydrogen‐bonded and hydrated Na + ion water (Figure 6a).…”

Section: Electro‐driven Water Splittingmentioning

confidence: 99%

Several Key Factors for Efficient Electrocatalytic Water Splitting: Active Site Coordination Environment, Morphology Changes and Intermediates Identification

Zhu

et al. 2022

Chemistry A European J

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Water-splitting has emerged as a promising alternative strategy to produce clean hydrogen fuel. However, current electrocatalytic water splitting suffers from sluggish kinetics, thus developing efficient electrocatalysts is crucial. Identifying reaction centers discloses the reaction mechanism and will undoubtedly facilitate the design and optimization of efficient water splitting electrocatalysts. This review summarizes several advances involving the identification of the actual active sites and intermediates capture on the catalytic surface. The morphology and valence states change on 2D materials are chose to illustrate how structural evolution affect catalytic activity. Specifically, in situ/ex situ electron microscopy techniques that used for the characterization of catalytic sites, and spectroscopy techniques that used to detect active intermediates at the molecular level are highlighted. In addition, several perspectives, such as the development of new in situ techniques and electrokinetic analysis methods, are emphasized to shed light on future research.

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“…Taking Au for HER as an example, the EDL geometry exhibits layerdependent orientation discrepancy of dipolar H 2 O molecules on the solution side (Figure 9a,b), which collectively vary from one-H-down to two-H-down configurations with increasing of the electric potential. [256,257] While for a compound-type catalyst, the dynamic charge transfer process is further complicated by physical property of the catalyst itself, intercalation versus de-intercalation of certain atomic species near the catalyst surface [258] and interfacial contact with the support. [259] Transition-metal phosphides such as Ni 5 P 4 and Fe 0.5 Co 0.5 P are promising catalysts owing to their high activity and multifunctionality in catalyzing chemical reactions.…”

Section: Topological Ferroelectric Metal Ni 2 Pmentioning

confidence: 99%

Progress on Emerging Ferroelectric Materials for Energy Harvesting, Storage and Conversion

Wei

Domingo

Sun

et al. 2022

Advanced Energy Materials

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Since the discovery of Rochelle salt a century ago, ferroelectric materials have been investigated extensively due to their robust responses to electric, mechanical, thermal, magnetic, and optical fields. These features give rise to a series of ferroelectric‐based modern device applications such as piezoelectric transducers, memories, infrared detectors, nonlinear optical devices, etc. On the way to broaden the material systems, for example, from three to two dimensions, new phenomena of topological polarity, improper ferroelectricity, magnetoelectric effects, and domain wall nanoelectronics bear the hope for next‐generation electronic devices. In the meantime, ferroelectric research has been aggressively extended to more diverse applications such as solar cells, water splitting, and CO2 reduction. In this review, the most recent research progress on newly emerging ferroelectric states and phenomena in insulators, ionic conductors, and metals are summarized, which have been used for energy storage, energy harvesting, and electrochemical energy conversion. Along with the intricate coupling between polarization, coordination, defect, and spin state, the exploration of transient ferroelectric behavior, ionic migration, polarization switching dynamics, and topological ferroelectricity, sets up the physical foundation ferroelectric energy research. Accordingly, the progress in understanding of ferroelectric physics is expected to provide insightful guidance on the design of advanced energy materials.

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In situ Raman spectroscopy reveals the structure and dissociation of interfacial water

Cited by 434 publications

References 34 publications

Unraveling the Electrocatalytic Reduction Mechanism of Enols on Copper in Aqueous Media

Unraveling the Electrocatalytic Reduction Mechanism of Enols on Copper in Aqueous Media

Several Key Factors for Efficient Electrocatalytic Water Splitting: Active Site Coordination Environment, Morphology Changes and Intermediates Identification

Progress on Emerging Ferroelectric Materials for Energy Harvesting, Storage and Conversion

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