S2- doping inducing self-adapting dual anion defects in ZnSn(OH)6 for highly efficient photoactivity

Chen, Bangfu; Meng, Zhongwei; Ouyang, Ping; Duan, Youyu; Li, Yuhan; Wang, Wanjun; Dong, Fan

doi:10.1016/j.apcatb.2023.123093

Cited by 16 publications

(6 citation statements)

References 76 publications

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“…Specifically, the stretching vibration characteristic peaks of the −OH group interacting with the methyl group of the catalyst (3229 cm –1 ) and the skeleton stretching vibrations of the aromatic ring (1610 cm –1 ) can be detected. Moreover, as the reaction progresses, the presence of benzaldehyde (1280 cm –1 ) , gradually diminishes, while the emergence of benzoic acid (1388 cm –1 ) and CO 2 (2306 cm –1 ) suggests the breakdown of short-chain carboxylate species into smaller inorganic molecules.…”

Section: Resultsmentioning

confidence: 99%

“…Specifically, the stretching vibration characteristic peaks of the −OH group interacting with the methyl group of the catalyst (3229 cm −1 ) 38 and the skeleton stretching vibrations of the aromatic ring (1610 cm −1 ) 13 can be detected. Moreover, as the reaction progresses, the presence of benzaldehyde (1280 cm −1 ) 13,36 gradually diminishes, while the emergence of benzoic acid (1388 cm −1 ) 19 and CO 2 (2306 cm −1 ) 37 suggests the breakdown of short-chain carboxylate species into smaller inorganic molecules. Furthermore, the dynamic evolution process of C 3 H 6 O adsorption and activation by ZHS-M was further investigated through in situ DRIFTS spectra experiments (Table S6).…”

Section: Identification Of Crucialmentioning

confidence: 99%

“…34 This observation leads us to infer that C 7 H 8 undergoes a weak oxidation reaction, even in the absence of light irradiation. Subsequently, the new absorption bands corresponding to the stretching vibrations of the aromatic ring skeleton (1610 cm −1 ), 13 benzyl alcohol (C 7 H 8 O) (1154 cm −1 ), 35 benzaldehyde (1280 cm −1 ), 32,36 benzoic acid (1388 cm −1 ), 19 and CO 2 (2306 cm −1 ) 37 can be well observed on the surface at the beginning of the photocatalytic oxidation reaction (Figure 3c). It should be noted that during the initial oxidation of C 7 H 8 , noticeable changes occur in the cumulative substances.…”

Section: Identification Of Crucialmentioning

confidence: 99%

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Synergistic Activation of Small Molecules and Free Radicals for the Deep Mineralization of Mixed VOCs

Chen,

Duan,

Chen

et al. 2024

ACS Catal.

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Deep mineralization of C 7 H 8 is often impeded by an ambiguous understanding of the key contributors to active species and the mechanism of benzene ring activation. Herein, the implementation of ZnSn(OH) 6 as a photocatalyst for the degradation of a mixture of C 7 H 8 and C 3 H 6 O aims to investigate the synergistic activation effects between small molecules and reactive free radicals. Upon irradiation, the catalyst exhibits a remarkable average decomposition efficiency of 98.42% toward the mixture (C 7 H 8 :C 3 H 6 O = 50:20 ppm), with a 97.8% degradation rate for C 7 H 8 and a 100% degradation rate for C 3 H 6 O. The molecular O 2 is the main active species for the photocatalytic oxidation of C 7 H 8 and C 3 H 6 O. Especially, activated C 7 H 8 and C 3 H 6 O undergo direct dehydrogenative cross-coupling in a radical state to produce the key intermediate C 10 H 12 O. Compared with the primary intermediate benzyl alcohol (ΔG = +1.52 eV), C 10 H 12 O (ΔG = −0.47 eV) displays a lower ring-opening energy barrier under • O 2− attack, thereby facilitating the selectivity of the photocatalytic oxidation ring-opening reaction of C 7 H 8 and the photodegradation of the mixture. The present research delves into the collaborative interplay between small molecules and reactive free radicals during the mineralization process of C 7 H 8 , thereby shedding light on innovative strategies for the efficient treatment of mixed polluted gases under real-world conditions.

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Section: Resultsmentioning

confidence: 99%

Section: Identification Of Crucialmentioning

confidence: 99%

Section: Identification Of Crucialmentioning

confidence: 99%

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Synergistic Activation of Small Molecules and Free Radicals for the Deep Mineralization of Mixed VOCs

Chen,

Duan,

Chen

et al. 2024

ACS Catal.

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“…[12] The Zn 2p orbital (Zn 2p 1/2 , 1044.8 eV; Zn 2p 3/2 , 1021.7 eV, Figure 2e) and Sn 3d orbital (Sn 3d 3/2 , 495.1 eV; Sn 3d 5/2 , 486.6 eV (Figure 2f) are attributed to Zn 2 + and Sn 4 + , respectively. At the same time, the characteristic peaks at 532.3 eV, 531.5 eV and 530.2 eV in the O 1s orbitals (Figure 2g), assignable to adsorbed H 2 O and hydroxyl species, chemisorbed oxygen and lattice oxygen, [13] respectively. However, as compared with the bare ZHS and single AlOOH, the corresponding area of adsorbed H 2 O and hydroxyl species in AZHS-20 decreases, indicative of the weak H 2 O absorption.…”

Section: Forschungsartikelmentioning

confidence: 89%

Water‐Resistance‐Based S‐Scheme Heterojunction for Deep Mineralization of Toluene

Li,

Chen,

Liu

et al. 2024

Angewandte Chemie

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Deep mineralization of low concentration toluene (C7H8) is one of the most significant but challenging reactions in photocatalysis. It is generally assumed that hydroxyl radicals (·OH) as the main reactive species contribute to the enhanced photoactivity, however, it remains ambiguous at this stage. Herein, a S‐scheme ZnSn(OH)6‐based heterojunction with AlOOH as water resistant surface layer is in situ designed for tuning the free radical species and achieving deep mineralization of C7H8. By employing a combination of in situ DRIFTS and materials characterization techniques, we discover that the dominant intermediates such as benzaldehyde and benzoic acid instead of toxic phenols are formed under the action of holes (h+) and superoxide radicals (·O2‐). These dominant intermediates turn out to greatly decrease the ring‐opening reaction barrier. This study offers new possibilities for rationally tailoring the active species and thus directionally producing dominant intermediates via designing water resistant surface layer.

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“…Meanwhile, BS-12 showed the same trend compared to pure BS (Figure S5a). 28,41 The optical bandgaps of as-prepared catalysts were calculated based on the Tauc equation. 26,42 Figure 4b shows that the bandgap (E g ) for pristine ZSH was 3.49 eV.…”

Section: Morphology and Chemical Compositionmentioning

confidence: 99%

Piezoelectric Polarization and Sulfur Vacancy Enhanced Photocatalytic Hydrogen Evolution Performance of Bi₂S₃/ZnSn(OH)₆ Piezo-photocatalyst

Li,

Zhu,

Huang

et al. 2024

Inorg. Chem.

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The combination of piezoelectric catalysis and photocatalysis could effectively enhance the carrier separation efficiency and further improve the hydrogen production activity. However, piezoelectric polarization always suffers from a low polarization strength, which severely restricts its actual applications. In this study, we successfully synthesized a novel sulfur vacancy-rich Bi 2 S 3 /ZnSn (OH) 6 (BS-12/ZSH) piezo-photocatalyst for hydrogen evolution through water splitting. Notably, the piezo-photocatalytic hydrogen generation rate of the 8% BS-12/ ZSH catalyst (336.21 μmol/g/h) was superior to that of pristine ZSH (29.71 μmol/g/h) and BS-12 (21.66 μmol/g/h). In addition, the hydrogen generation for 8% BS-12/ZSH (336.21 μmol/g/h) under ultrasonic coupling illumination was significantly higher than that under single illumination (52.09 μmol/g/h) and ultrasound (121.90 μmol/g/h), owing to the cooperative interaction of the sulfur vacancy and piezoelectric field. Various characterization analyses confirmed that (1) the introduction of sulfur vacancies in BS-12 provided more active sites, (2) BS-12 with sulfur vacancies acted as a co-catalyst to accelerate the hydrogen production rate, and (3) the piezoelectric field eliminated the electrostatic shielding and offered an additional driving force, which effectively promoted the separation of electron−hole pairs. This research clearly reveals the synergistic effect between piezocatalysis and photocatalysis as well as offers a promising sight for the rational design of high-efficiency piezo-photocatalysts.

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S2- doping inducing self-adapting dual anion defects in ZnSn(OH)6 for highly efficient photoactivity

Cited by 16 publications

References 76 publications

Synergistic Activation of Small Molecules and Free Radicals for the Deep Mineralization of Mixed VOCs

Synergistic Activation of Small Molecules and Free Radicals for the Deep Mineralization of Mixed VOCs

Water‐Resistance‐Based S‐Scheme Heterojunction for Deep Mineralization of Toluene

Piezoelectric Polarization and Sulfur Vacancy Enhanced Photocatalytic Hydrogen Evolution Performance of Bi₂S₃/ZnSn(OH)₆ Piezo-photocatalyst

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S2- doping inducing self-adapting dual anion defects in ZnSn(OH)6 for highly efficient photoactivity

Cited by 16 publications

References 76 publications

Synergistic Activation of Small Molecules and Free Radicals for the Deep Mineralization of Mixed VOCs

Synergistic Activation of Small Molecules and Free Radicals for the Deep Mineralization of Mixed VOCs

Water‐Resistance‐Based S‐Scheme Heterojunction for Deep Mineralization of Toluene

Piezoelectric Polarization and Sulfur Vacancy Enhanced Photocatalytic Hydrogen Evolution Performance of Bi2S3/ZnSn(OH)6 Piezo-photocatalyst

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Piezoelectric Polarization and Sulfur Vacancy Enhanced Photocatalytic Hydrogen Evolution Performance of Bi₂S₃/ZnSn(OH)₆ Piezo-photocatalyst