Enhanced localized dipole of Pt-Au single-site catalyst for solar water splitting

Liu, Xingyu; Hao, Zhineng; Wang, Haitao; Wang, Tuo; Shen, Zhurui; Zhang, Hao; Zhan, Sihui; Gong, Jinlong

doi:10.1073/pnas.2119723119

Cited by 26 publications

(27 citation statements)

References 54 publications

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“…As shown from the LSV curves in Figure a, a potential of 1.8 V sustained a current density ( j ) of 80.3 mA cm –2 for Ti/RuO 2 needles, which was in sharp contrast to the values of 52.4 and 23.4 mA cm –2 obtained from the Ti/RuO 2 rods and slab. Electrochemical impedance spectroscopy (EIS) verified the faster charge-transfer kinetics by the high-curvature nanostructure (Figure c), with the charge-transfer resistance ( R ct ) in the Ti/RuO 2 needles being approximately 30 Ω, much smaller than the R ct value of 45 Ω for the Ti/RuO 2 rods and 65 Ω for the Ti/RuO 2 slab, which indicated effective electron transfer induced by the tip-enrichment effect …”

Section: Results and Discussionmentioning

confidence: 99%

“…Electrochemical impedance spectroscopy (EIS) verified the faster charge-transfer kinetics by the high-curvature nanostructure (Figure 2c), with the charge-transfer resistance (R ct ) in the Ti/RuO 2 needles being approximately 30 Ω, much smaller than the R ct value of 45 Ω for the Ti/RuO 2 rods and 65 Ω for the Ti/RuO 2 slab, which indicated effective electron transfer induced by the tipenrichment effect. 20 The AC generation measured in 0.5 M NaCl of pH 6 quantified FE for Ti/RuO 2 needles was 47.6%, which was 23.6 and 47.5% higher than that of Ti/RuO 2 rods and slab, respectively. The effect of potential on the efficiency of AC generation was demonstrated in Figure S2, revealing that the FEs were 54.3, 65.2, 55.9, and 44.6% at 1.6, 2.0, 2.4, and 2.8 V, respectively.…”

Section: ■ Introductionmentioning

confidence: 99%

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Tip-Intensified Interfacial Microenvironment Reconstruction Promotes an Electrocatalytic Chlorine Evolution Reaction

et al. 2022

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Electrocatalysis applied in energy conversions has recently been associated with nanotips that catalyze extensive fuelforming or value-adding reactions. However, the enhanced catalytic behavior governed by tip-intensified microenvironment reconstruction is particularly elusive and is yet to be understood. Here, we demonstrated a homemade visualization platform to collect information from the local microenvironment of a solution near an electrode (LMSE) with high temporal−spatial resolution, thereby figuring out the sharp-tip enhancement effect for the chlorine evolution reaction (CER). Through visualization using sensitive Cl − and pH sensors, we confirmed that periodic nanoneedles were beneficial for field-induced anion concentration, giving priority to water dissociation and synchronously creating optimal pH conditions for triggering the CER, whereby the Cl − consumption rate within the LMSE was 1.3 times higher than that of the slab counterpart. Tip-enhanced effects meanwhile endowed the local microenvironment with intensified concentration and temperature gradients for continuous transport of Cl − substrates and effective diffusion of HClO products, whereby the oxygen evolution reaction for persistent CER activities was restrained. Our study provides definitive evidence that the optimal microenvironment functionalized with tip-intensified ion concentration from the electrolyte and water dissociation at tip sites are key to stabilize the crucial reaction intermediate for superior electrocatalytic performance.

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Section: Results and Discussionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Tip-Intensified Interfacial Microenvironment Reconstruction Promotes an Electrocatalytic Chlorine Evolution Reaction

et al. 2022

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“…Nevertheless, single atoms may not significantly change the charge transfer process of photocatalysts, so it is difficult to promote the charge separation and migration, which extremely limits the promoting effects of single-atom doping on the photocatalysis of 2D materials. 39,40 As we all know, the dipole with a positive center and a negative center is the elementary entity of the electric field and the major driving force of charge separation and migration. Inspired by this, we synthesized the ultrathin g-C 3 N 4 nanosheets loaded with a Pt−Au binary single atom (Pt−Au SAC) (Figure 6a,b).…”

Section: Single-metal-atom Loadingmentioning

confidence: 99%

“…Furthermore, because of their unique electronic and geometric structure, single atoms could promote the photocatalytic activity primarily through optimizing the surface chemical reactions caused by charge evolution, such as reactant adsorption or charge migration from photocatalysts to reactants. Nevertheless, single atoms may not significantly change the charge transfer process of photocatalysts, so it is difficult to promote the charge separation and migration, which extremely limits the promoting effects of single-atom doping on the photocatalysis of 2D materials. , …”

Section: Modulation Strategy Of Inorganic Ultrathin Two-dimensional N...mentioning

confidence: 99%

“…As we all know, the dipole with a positive center and a negative center is the elementary entity of the electric field and the major driving force of charge separation and migration. Inspired by this, we synthesized the ultrathin g-C 3 N 4 nanosheets loaded with a Pt–Au binary single atom (Pt–Au SAC) (Figure a,b) . EXAFS spectra (Figure c,d) and DFT calculation (Figure e) show that the platinum and gold atoms in Pt–Au SAC and Au single-site counterparts (Au SAC) tend to stabilize in the hexaploid cavities between heptazine subunits (with Pt–N 4 /Au–N 5 coordination), while the platinum atoms in platinum single-site counterparts (Pt SAC) tend to occupy the carbon vacancies (with Pt–N 3 coordination).…”

Section: Modulation Strategy Of Inorganic Ultrathin Two-dimensional N...mentioning

confidence: 99%

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Inorganic Ultrathin 2D Photocatalysts: Modulation Strategies and Environmental/Energy Applications

Zhang

Zhao

et al. 2022

Acc. Mater. Res.

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Metrics & MoreArticle Recommendations * sı Supporting Information CONSPECTUS: Photocatalysis technology has gained extensive attention in the past few decades due to its potential to alleviate or solve energy and environmental contamination problems. The development and design of new photocatalytic semiconductor materials with high catalytic activity has become a research hotspot in this field. In recent years, inorganic ultrathin two-dimensional (2D) semiconductor photocatalysts have shown excellent performance in photocatalytic applications due to their high specific surface area, clear atomic structure, unique electronic structure, intrinsic quantum confined electrons, and high atomic exposure ratio. When the thickness of the bulk semiconductor is decreased to the atomic level, its local atomic structure changes prominently. This is a major reason why the atomic thin 2D materials could show improved inherent properties and produce new properties that are not available in the corresponding bulk semiconductors. Furthermore, compared with the bulk photocatalysts, the surface electronic structure of inorganic ultrathin 2D materials is more sensitive and thus could be regulated more easily by surface and interfacial modification methods, leading to great optimization of photocatalytic properties. Therefore, inorganic ultrathin 2D materials not only provide an ideal reaction model for clearly revealing the relationships between surface/interface structure characteristics and photocatalytic performance but also bring new opportunities for the development of efficient catalysts to resolve energy crises and environmental problems.In this Account, we summarize our previous work on the applications of inorganic ultrathin 2D nanomaterials in the field of photocatalysis. First, we briefly introduce the classification and controlled fabrication of inorganic ultrathin 2D nanomaterials, including metal chalcogenides, bismuth-based photocatalysts, metal oxides, and metal-free materials. Then, we focus on the surface and interfacial modification strategies for effectively engineering the photocatalytic activity of 2D photocatalysts, including defect engineering, metal doping, single atom loading, and heterojunction construction. These strategies can effectively adjust the inherent physical and chemical properties of inorganic ultrathin 2D nanomaterials, change their electronic structure to improve the light absorption ability, promote the separation and migration of photogenerated electrons and holes, optimize the catalytic active sites, and even change the reaction energy barrier of the photocatalytic reaction. Additionally, we discuss the research progress of inorganic ultrathin 2D photocatalysts in hydrogen evolution, contaminant removal, and sterilization. Finally, we put forward the prospects, challenges, and novel viewpoints of feasible solutions of inorganic ultrathin 2D materials in photocatalysis applications.Overall, this Account provides in-depth insight into modulation strategies and the structure−activity relations...

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Integrating Mixed Halide Perovskite Photocatalytic HI Splitting and Electrocatalysis into a Loop for Efficient and Robust Pure Water Splitting

et al. 2023

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Developing a hydrogen economy to replace traditional fossil fuels is essential for sustainable human development. As two promising H2 production strategies, photocatalytic and electrocatalytic water splitting with large reaction energy barriers still face the great challenges of poor solar‐to‐hydrogen efficiency and large electrochemical overpotentials, respectively. Herein, a new strategy is proposed to disassemble the difficult pure water splitting into two parts that are easy to implement, namely mixed halide perovskite photocatalytic HI splitting for H2 production, and simultaneous electrocatalytic I3− reduction and O2 production. The efficient charge separation, abundant H2 production active sites, and a small HI splitting energy barrier contribute to the superior photocatalytic H2 production activity of MoSe2/MAPbBr3−xIx (CH3NH3+ = MA). Subsequent electrocatalytic I3− reduction and O2 production reactions only need a small voltage of 0.92 V to drive, which is far lower than that of the electrocatalytic pure water splitting (>1.23 V). The molar ratio of H2 (6.99 mmol g−1) to O2 (3.09 mmol g−1) produced during the first photocatalytic and electrocatalytic cycle is close to 2:1, and the continuous circulation of I3−/I− between the photocatalytic and electrocatalytic systems can achieve efficient and robust pure water splitting.

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Enhanced localized dipole of Pt-Au single-site catalyst for solar water splitting

Cited by 26 publications

References 54 publications

Tip-Intensified Interfacial Microenvironment Reconstruction Promotes an Electrocatalytic Chlorine Evolution Reaction

Tip-Intensified Interfacial Microenvironment Reconstruction Promotes an Electrocatalytic Chlorine Evolution Reaction

Inorganic Ultrathin 2D Photocatalysts: Modulation Strategies and Environmental/Energy Applications

Integrating Mixed Halide Perovskite Photocatalytic HI Splitting and Electrocatalysis into a Loop for Efficient and Robust Pure Water Splitting

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