Gold–nickel phosphide heterostructures for efficient photocatalytic hydrogen peroxide production from real seawater

Wang, Ning; Wang, Wei; Luo, Qi; Li, Jinyang; Li, Yunhong; Li, Linqian; Huo, Xiaobing; Du, Xi‐Wen

doi:10.1039/d2qi02662g

Cited by 8 publications

(2 citation statements)

References 59 publications

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“…It is worth mentioning that 97% of the entire water on Earth is seawater and only 3% is fresh water. The presence of various salts in seawater often leads to the deactivation of the photocatalysts, thus limiting their practical application. , While some signs of progress have been achieved in electrocatalysis, the photocatalytic approach is still in its infancy, ,− and still no report exists on SAC-based photocatalysts using seawater to produce H 2 O 2 .…”

Section: Introductionmentioning

confidence: 99%

An Atomically Dispersed Mn-Photocatalyst for Generating Hydrogen Peroxide from Seawater via the Water Oxidation Reaction (WOR)

et al. 2023

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In this work, we have fabricated an aryl amino-substituted graphitic carbon nitride (g-C 3 N 4 ) catalyst with atomically dispersed Mn capable of generating hydrogen peroxide (H 2 O 2 ) directly from seawater. This new catalyst exhibited excellent reactivity, obtaining up to 2230 μM H 2 O 2 in 7 h from alkaline water and up to 1800 μM from seawater under identical conditions. More importantly, the catalyst was quickly recovered for subsequent reuse without appreciable loss in performance. Interestingly, unlike the usual two-electron oxygen reduction reaction pathway, the generation of H 2 O 2 was through a less common two-electron water oxidation reaction (WOR) process in which both the direct and indirect WOR processes occurred; namely, photoinduced h + directly oxidized H 2 O to H 2 O 2 via a one-step 2e − WOR, and photoinduced h + first oxidized a hydroxide (OH − ) ion to generate a hydroxy radical ( • OH), and H 2 O 2 was formed indirectly by the combination of two • OH. We have characterized the material, at the catalytic sites, at the atomic level using electron paramagnetic resonance, X-ray absorption near edge structure, extended X-ray absorption fine structure, high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, magic-angle spinning solid-state NMR spectroscopy, and multiscale molecular modeling, combining classical reactive molecular dynamics simulations and quantum chemistry calculations.

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Section: Introductionmentioning

confidence: 99%

An Atomically Dispersed Mn-Photocatalyst for Generating Hydrogen Peroxide from Seawater via the Water Oxidation Reaction (WOR)

et al. 2023

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“…[1][2][3][4] Meanwhile, H 2 O 2 is also a potential liquid carbon-neutral energy carrier to replace fossil fuels in terms of sustainability, renewability, high energy density, and low-cost transportation. [5][6][7][8] Currently, the industrial production of H 2 O 2 relies on environmentally hazardous and energy-consuming anthraquinone technology. [9][10][11] By comparison, harvesting sunlight DOI: 10.1002/smll.202301865 by an active semiconductor for the reductive transformation of O 2 into H 2 O 2 has been regarded as a sustainable and promising pathway to yield H 2 O 2 without discharging any hazardous chemicals.…”

Section: Introductionmentioning

confidence: 99%

Solar‐Driven Production Of Hydrogen Peroxide And Benzaldehyde In Two‐Phase System By An Interface‐Engineered Co₉S₈‐CoZnIn₂S₄ Heterostructure

Huo

Chen

et al. 2023

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Coupling the photoproduction of solar fuel and value‐added chemicals is highly attractive, as it maximizes the utilization of incident sunlight and the economic value of photocatalytic reactions. Constructing intimate semiconductor heterojunction for these reactions is highly desirable due to accelerated charge separation at the interfacial contact, but is challenged by material synthesis. Here, an active heterostructure bearing intimate interface, consisting of discrete Co9S8 nanoparticles anchored on cobalt doped ZnIn2S4 using a facile in situ one‐step strategy, can drive photocatalytic co‐production of H2O2 and benzaldehyde from a two‐phase water/benzyl alcohol system with spatial product separation is reported. The heterostructure yields a high production amount of 49.5 and 55.8 mmol L−1 for H2O2 and benzaldehyde under visible‐light soaking, respectively. The synchronous elemental Co doping and intimate heterostructure establishment substantially improve the overall reaction kinetics. Mechanism studies reveal that H2O2 generated in the aqueous phase undergoes photodecomposition forming hydroxyl radical, which is subsequently transferred into the organic phase to oxidize benzyl alcohol into benzaldehyde. This study offers fertile guidelines for creating integrated semiconductors and broadens the avenue toward the coupled production of solar fuels and industrially important chemicals.

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Covalent Organic Frameworks with Constrained Palladium Nanoclusters Lock the Enol‐Keto Tautomerism Enhancing Hydrogen Peroxide Photosynthesis

Zhou,

Chen,

et al. 2024

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The production of hydrogen peroxide from natural seawater is green and sustainable. However, the efficiency of photocatalytic hydrogen peroxide production is low due to the degradation and poisoning of photocatalysts by the abundant ions in natural seawater. Precisely controlling the structure of photocatalysts to enhance their corrosion resistance and minimize the impact of external particles is a challenging task. Here, a novel molecular engineering strategy is reported in which confined Pd nanoclusters locked keto structures to enhance photocatalytic hydrogen peroxide production. Both experimental and theoretical findings reveals that Pd nanoclusters, when confined within a keto structure, not only bolster the stability of the photocatalyst but also augment the efficiency of photogenerated charge carriers' separation and transport. This dual enhancement significantly boosts the photocatalytic performance for hydrogen peroxide synthesis. One of the photocatalysts, TAPT‐2KtTb Pd COF, exhibits an impressive photocatalytic hydrogen peroxide production rate of 2676.3 µmol g−1 h−1, which is one of the highest values reported so far. Integral photocatalyzed H2O2 synthesis using confined Pd nanoclusters locked keto conformation COF provides a new insight for developing innovative photocatalysts for H2O2 synthesis.

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Gold–nickel phosphide heterostructures for efficient photocatalytic hydrogen peroxide production from real seawater

Abstract: Direct hydrogen peroxide (H2O2) photosynthesis from earth-abundant seawater provides an attractive path for scalable and cost-effective solar fuel production for the future, but the sluggish half-reaction of water oxidation and...

Cited by 8 publications

References 59 publications

An Atomically Dispersed Mn-Photocatalyst for Generating Hydrogen Peroxide from Seawater via the Water Oxidation Reaction (WOR)

An Atomically Dispersed Mn-Photocatalyst for Generating Hydrogen Peroxide from Seawater via the Water Oxidation Reaction (WOR)

Solar‐Driven Production Of Hydrogen Peroxide And Benzaldehyde In Two‐Phase System By An Interface‐Engineered Co₉S₈‐CoZnIn₂S₄ Heterostructure

Covalent Organic Frameworks with Constrained Palladium Nanoclusters Lock the Enol‐Keto Tautomerism Enhancing Hydrogen Peroxide Photosynthesis

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Gold–nickel phosphide heterostructures for efficient photocatalytic hydrogen peroxide production from real seawater

Abstract: Direct hydrogen peroxide (H2O2) photosynthesis from earth-abundant seawater provides an attractive path for scalable and cost-effective solar fuel production for the future, but the sluggish half-reaction of water oxidation and...

Cited by 8 publications

References 59 publications

An Atomically Dispersed Mn-Photocatalyst for Generating Hydrogen Peroxide from Seawater via the Water Oxidation Reaction (WOR)

An Atomically Dispersed Mn-Photocatalyst for Generating Hydrogen Peroxide from Seawater via the Water Oxidation Reaction (WOR)

Solar‐Driven Production Of Hydrogen Peroxide And Benzaldehyde In Two‐Phase System By An Interface‐Engineered Co9S8‐CoZnIn2S4 Heterostructure

Covalent Organic Frameworks with Constrained Palladium Nanoclusters Lock the Enol‐Keto Tautomerism Enhancing Hydrogen Peroxide Photosynthesis

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Solar‐Driven Production Of Hydrogen Peroxide And Benzaldehyde In Two‐Phase System By An Interface‐Engineered Co₉S₈‐CoZnIn₂S₄ Heterostructure