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学者姓名：徐艺军
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Abstract ：
Switchable divergent organic transformations represent a straightforward but challenging method to synthesize structurally varied compounds starting from the same set of raw materials. Herein, we report the divergent dehydrocoupling of thiols into tunable disulfides/thioethers and H2 in response to the visible or ultraviolet (UV) light, over CdS quantum dots. Regulating the irradiation wavelength allows disulfides and thioethers to be synthesized in moderate to high yields with good functional group tolerance. Mechanistic studies reveal that thiols are oxidized to produce sulfur-centered radicals by photogenerated holes under visible light irradiation, which then undergo S-S coupling to form disulfides. While under UV light irradiation, the cleavage of C-S bonds in thiols occurs readily to afford aryl radicals, which interact with sulfur-centered radicals, undergoing C-S coupling to obtain thioethers. This work is expected to open an avenue of light-controlled switch to maneuver a radical conversion route for divergent synthesis of value-added fine chemicals.
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| GB/T 7714 | Qi, Ming-Yu , Shao, Xin-Ni , Tang, Zi-Rong et al. Light-Controlled Switch for Divergent Coupling of Thiols to Disulfides/Thioethers over CdS Quantum Dots [J]. | ACS MATERIALS LETTERS , 2025 , 7 (4) : 1533-1539 . |
| MLA | Qi, Ming-Yu et al. "Light-Controlled Switch for Divergent Coupling of Thiols to Disulfides/Thioethers over CdS Quantum Dots" . | ACS MATERIALS LETTERS 7 . 4 (2025) : 1533-1539 . |
| APA | Qi, Ming-Yu , Shao, Xin-Ni , Tang, Zi-Rong , Xu, Yi-Jun . Light-Controlled Switch for Divergent Coupling of Thiols to Disulfides/Thioethers over CdS Quantum Dots . | ACS MATERIALS LETTERS , 2025 , 7 (4) , 1533-1539 . |
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The development of photocatalytic systems that enable the simultaneous production of H2O2 and value-added organic chemicals presents a dual advantage: generating valuable products while maximizing the utilization of solar energy. Despite the potential, there are relatively few reports on photocatalysts capable of such dual functions. In this study, we synthesized a series of donor-acceptor covalent organic frameworks (COFs), designated as JUC-675 to JUC-677, to explore their photocatalytic efficiency in the co-production of H2O2 and N-benzylbenzaldimine (BBAD). Among them, JUC-675 exhibited exceptional performance, achieving a H2O2 production rate of 22.8 mmol g(-1) h(-1) with an apparent quantum yield of 15.7 %, and its solar-to-chemical conversion efficiency was calculated to be 1.09 %, marking it as the most effective COF-based photocatalyst reported to date. Additionally, JUC-675 demonstrated a high selectivity (99.9 %) and yield (96 %) for BBAD in the oxidative coupling of benzylamine. The underlying reaction mechanism was thoroughly investigated through validation experiments and density functional theory (DFT) calculations. This work represents a significant advancement in the design of COF-based photocatalysts and the development of efficient dual-function photocatalytic platforms, offering new insights and methodologies for enhanced solar energy utilization and the synthesis of value-added products.
Keyword ：
co-production systems co-production systems covalent organic frameworks covalent organic frameworks H2O2 production H2O2 production oxidative organic transformations oxidative organic transformations photocatalytic photocatalytic
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| GB/T 7714 | Liu, Jianchuan , Tuo, Chao , Xiao, Wei-Yun et al. Constructing Donor-Acceptor Covalent Organic Frameworks for Highly Efficient H2O2 Photosynthesis Coupled with Oxidative Organic Transformations [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (9) . |
| MLA | Liu, Jianchuan et al. "Constructing Donor-Acceptor Covalent Organic Frameworks for Highly Efficient H2O2 Photosynthesis Coupled with Oxidative Organic Transformations" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 9 (2025) . |
| APA | Liu, Jianchuan , Tuo, Chao , Xiao, Wei-Yun , Qi, Ming-Yu , Yusran, Yusran , Wang, Zitao et al. Constructing Donor-Acceptor Covalent Organic Frameworks for Highly Efficient H2O2 Photosynthesis Coupled with Oxidative Organic Transformations . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (9) . |
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Cooperatively integrating CO2 reduction half-reaction with selective organic oxidation half-reaction presents an attractive opportunity to simultaneously utilize photogenerated holes and electrons to realize carbon neutrality and the production of value-added chemicals. Herein, we report the cooperative photoredox catalysis of tunable and efficient CO2 reduction to syngas paired with 4-methoxythiophenol (4-MTP) oxidation to bis(4methoxyphenyl) disulfide (4-MPD) over hybrid CdSe/CdS quantum dots (QDs). The strategy of constructing CdSe/CdS composites not only facilitates the efficiency of photoinduced carrier separation and transfer, improving the photoredox activity of two half-reactions, but also enhances CO2 activation, modulating the syngas CO/H2 ratio varying from 1:4-5:4. Mechanistic studies have revealed that 4-MTP is oxidized by holes located in CdS to generate hydrogen protons and sulfur-centered radicals, and then these radicals pair with each other to form 4-MPD with high selectivity, while the electrons in CdSe interact with protons and CO2 for syngas production. Furthermore, the feasibility of applying CdSe/CdS QDs to the cooperative photoredox catalysis of thiols with different substituents integrated with CO2 into corresponding disulfides and syngas has been demonstrated. This work envisages the development of QDs-based heterostructure catalysts for highly efficient photocatalytic co-production of syngas and value-added organic chemicals.
Keyword ：
CdSe/CdS QDs CdSe/CdS QDs CO 2 reduction CO 2 reduction Disulfides Disulfides Syngas Syngas Thiols oxidation Thiols oxidation
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| GB/T 7714 | Zhang, Yi , Gao, Long-Hui , Qi, Ming-Yu et al. Cooperative photoredox coupling of CO2 reduction with thiols oxidation by hybrid CdSe/CdS semiconductor quantum dots [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2025 , 367 . |
| MLA | Zhang, Yi et al. "Cooperative photoredox coupling of CO2 reduction with thiols oxidation by hybrid CdSe/CdS semiconductor quantum dots" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 367 (2025) . |
| APA | Zhang, Yi , Gao, Long-Hui , Qi, Ming-Yu , Tang, Zi-Rong , Xu, Yi-Jun . Cooperative photoredox coupling of CO2 reduction with thiols oxidation by hybrid CdSe/CdS semiconductor quantum dots . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2025 , 367 . |
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Light-driven photoredox catalysis presents a promising approach for the activation and conversion of methane (CH4) into high value-added chemicals under ambient conditions. However, the high C-H bond dissociation energy of CH4 and the absence of well-defined C-H activation sites on catalysts significantly limit the highly efficient conversion of CH4 toward multicarbon (C2+) hydrocarbons, particularly ethylene (C2H4). Herein, we demonstrate a bimetallic design of Ag nanoparticles (NPs) and Pd single atoms (SAs) on ZnO for the cascade conversion of CH4 into C2H4 with the highest production rate compared with previous works. Mechanistic studies reveal that the synergistic effect of Ag NPs and Pd SAs, upon effecting key bond-breaking and -forming events, lowers the overall energy barrier of the activation process of both CH4 and the resulting C2H6, constituting a truly synergistic catalytic system to facilitate the C2H4 generation. This work offers a novel perspective on the advancement of photocatalytic directional CH4 conversion toward high value-added C2+ hydrocarbons through the subtle design of bimetallic cascade catalyst strategy. We present a bimetallic design of Ag nanoparticles (NPs) and Pd single atoms (SAs) on ZnO for the cascade photocatalytic CH4 conversion toward C2H4 with the highest production rate compared with previous works. The synergistic effect of Ag NPs and Pd SAs lowers the overall energy barrier of the activation process of both CH4 and the resulting C2H6, constituting a truly synergistic catalytic system to facilitate the C2H4 generation. image
Keyword ：
bimetallic sites bimetallic sites C-H activation C-H activation ethylene ethylene methane conversion methane conversion photocatalysis photocatalysis
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| GB/T 7714 | Wang, Yin-Feng , Qi, Ming-Yu , Conte, Marco et al. Bimetallic Single Atom/Nanoparticle Ensemble for Efficient Photochemical Cascade Synthesis of Ethylene from Methane [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (34) . |
| MLA | Wang, Yin-Feng et al. "Bimetallic Single Atom/Nanoparticle Ensemble for Efficient Photochemical Cascade Synthesis of Ethylene from Methane" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 34 (2024) . |
| APA | Wang, Yin-Feng , Qi, Ming-Yu , Conte, Marco , Tang, Zi-Rong , Xu, Yi-Jun . Bimetallic Single Atom/Nanoparticle Ensemble for Efficient Photochemical Cascade Synthesis of Ethylene from Methane . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (34) . |
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Janus heterostructures consisting of multiple jointed components with distinct properties have gained growing interest in the photoredox catalytic field. Herein, we have developed a facile low-temperature method to gain anisotropic one-dimensional Au-tipped CdS (Au-CdS) nanorods (NRs), followed by assembling Ru molecular co-catalyst (RuN5) onto the surface of the NRs. The CdS NRs decorated with plasmonic Au nanoparticles (NPs) and RuN5 complex harness the virtues of metal-semiconductor and inorganic-organic interface, giving directional charge transfer channels, spatially separated reaction sites, and enhanced local electric field distribution. As a result, the Au-CdS-RuN5 can act as an efficient dual-function photocatalyst for simultaneous H2 evolution and valorization of biomass-derived alcohols. Benefiting from the interfacial charge decoupling and selective chemical bond activation, the optimal all-in-one Au-CdS-RuN5 heterostructure shows greatly enhanced photoactivity and selectivity as compared to bare CdS NRs, along with a remarkable apparent quantum yield of 40.2 % at 400 nm. The structural evolution and working mechanism of the heterostructures are systematically analyzed based on experimental and computational results. We report the design of a reduction co-catalyst-tipped and oxidation co-catalyst-capped Janus heterostructure, which reveals the benefits of efficient interfacial charge separation via transfer of photogenerated electrons and holes, respectively, to Au and RuN5 sites for selective organic synthesis and H2 production via photoredox paired reaction coupling. image
Keyword ：
charge decoupling charge decoupling dual-function catalyst dual-function catalyst functional active site functional active site Janus structure Janus structure selective photoredox selective photoredox
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| GB/T 7714 | Han, Chuang , Zeng, Zikang , Zhang, Xiaorui et al. All-in-One: Plasmonic Janus Heterostructures for Efficient Cooperative Photoredox Catalysis [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (38) . |
| MLA | Han, Chuang et al. "All-in-One: Plasmonic Janus Heterostructures for Efficient Cooperative Photoredox Catalysis" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 38 (2024) . |
| APA | Han, Chuang , Zeng, Zikang , Zhang, Xiaorui , Liang, Yujun , Kundu, Bidyut Kumar , Yuan, Lan et al. All-in-One: Plasmonic Janus Heterostructures for Efficient Cooperative Photoredox Catalysis . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (38) . |
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The valorization of lignocellulosic biomass represents a significant frontier in scientific research, promising a sustainable source of renewable energy and valuable chemical compounds. Traditional methods for converting lignocellulose often suffer from challenges such as low selectivity, suboptimal yield, and high energy consumption. To address these issues, innovative approaches that blend different catalytic processes are gaining traction. One such approach is the combination of sonication with photocatalysis in continuous-flow systems. This method offers the potential to revolutionize lignocellulose valorization by enhancing process efficiency and selectivity, thus opening new pathways for producing high-value chemicals and energy sources. This paper delves into the potential of integrating sonication and photocatalysis for lignocellulose conversion within continuous-flow systems. It discusses the opportunities that arise from this synergistic approach, as well as the associated challenges, such as the need for precise control of reaction conditions and the integration of scalable technologies. Moreover, a critical review of the current state of the art in this domain is provided to highlight recent advancements and identify avenues for future exploration. This paper is particularly relevant to researchers, engineers, and professionals in chemical engineering, renewable energy, and environmental science who are focused on sustainable technologies and biomass conversion. It is also valuable for academic and industrial stakeholders seeking innovative solutions to enhance the efficiency and sustainability of biomass processing.
Keyword ：
Continuous-flow processes Continuous-flow processes Hydrogen production Hydrogen production Lignocellulose valorization Lignocellulose valorization Renewable energy Renewable energy Sono-Photocatalysis Sono-Photocatalysis
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| GB/T 7714 | Hosseini, Behdokht Hashemi , Paszkiewicz-Gawron, Marta , Varma, Rajender S. et al. Sono-photocatalysis for continuous-flow intensification: A disruptive strategy for lignocellulose valorization [J]. | APPLIED CATALYSIS O: OPEN , 2024 , 193 . |
| MLA | Hosseini, Behdokht Hashemi et al. "Sono-photocatalysis for continuous-flow intensification: A disruptive strategy for lignocellulose valorization" . | APPLIED CATALYSIS O: OPEN 193 (2024) . |
| APA | Hosseini, Behdokht Hashemi , Paszkiewicz-Gawron, Marta , Varma, Rajender S. , Xu, Yi-Jun , Hsu, Hsien-Yi , Quintero, Juan Carlos Colmenares . Sono-photocatalysis for continuous-flow intensification: A disruptive strategy for lignocellulose valorization . | APPLIED CATALYSIS O: OPEN , 2024 , 193 . |
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Visible light induced oxidative C-C and C-N coupling provides a milder alternative to the current synthetic strategies. However, the photochemical C-C coupling of benzylamine and chromoselective C-C/C-N conversion are not widely reported. Herein, we demonstrate that the introduction of indium vacancies in ZnIn2S4 improves the catalytic activity for C-C coupling of benzylamine and imparts a strong chromoselectivity for C-C or C-N coupled products. A high C-C selectivity of similar to 80% is achieved with a benzylamine conversion of similar to 80%. Mechanistic studies unveil the switchable reaction routes between kinetically favored C-C coupling and thermodynamically favored C-N coupling under specific illumination conditions.
Keyword ：
C-Cbond formation C-Cbond formation C-N bond formation C-N bond formation defect engineering defect engineering photocatalytic photocatalytic wavelength selective wavelength selective ZnIn2S4 ZnIn2S4
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| GB/T 7714 | Leng, Xiaohui , Zhou, Xin , Ma, Lu et al. Wavelength-Selective C-C and C-N Bond Formation via Defect-Engineered ZnIn2S4 [J]. | ACS CATALYSIS , 2024 , 14 (15) : 11554-11563 . |
| MLA | Leng, Xiaohui et al. "Wavelength-Selective C-C and C-N Bond Formation via Defect-Engineered ZnIn2S4" . | ACS CATALYSIS 14 . 15 (2024) : 11554-11563 . |
| APA | Leng, Xiaohui , Zhou, Xin , Ma, Lu , Du, Yonghua , Peng, Ouwen , Chen, Zhongxin et al. Wavelength-Selective C-C and C-N Bond Formation via Defect-Engineered ZnIn2S4 . | ACS CATALYSIS , 2024 , 14 (15) , 11554-11563 . |
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Utilizing semiconductor quantum dots (QDs) to construct a bifunctional reaction system of coupling CO2 reduction with biomass valorization represents an appealing approach for the production of useable fuels and value-added chemicals. Herein, we present an efficient cooperative photocatalytic process for simultaneously achieving the reduction of CO2 to syngas and the oxidation of biomass-derived furfuryl alcohol to furfural and hydrofuroin over SiO2-supported CdSe/CdS QDs (CdSe/CdS-SiO2). The type-II band alignment in CdSe/CdS core/shell heterostructures enables effective charge separation and interfacial charge migration concurrently. By further assembly onto a spherical SiO2 support, the optimized CdSe/CdS-SiO2 composite exhibits remarkably enhanced activities for syngas and furfural/hydrofuroin production, which are 2.3 and 3.5 times higher than those of binary CdSe/CdS core/shell QDs, and 90.4 and 18.5 times higher than those of bare CdSe QDs, along with good stability. In particular, by altering the thickness of the CdS shell, the syngas CO/H-2 ratio can be precisely modulated within a wide range (1.6 to 7.1), which serves as crucial feedstock for the production of liquid fuels. This work is expected to develop core/shell QD-based photocatalysts for versatile and available photoredox-catalyzed reaction systems that integrate CO2 valorization with biomass upgrading.
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| GB/T 7714 | Zhang, Lin-Xing , Tang, Zi-Rong , Qi, Ming-Yu et al. Engineering semiconductor quantum dots for co-upcycling of CO2 and biomass-derived alcohol [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2024 , 12 (30) : 19029-19038 . |
| MLA | Zhang, Lin-Xing et al. "Engineering semiconductor quantum dots for co-upcycling of CO2 and biomass-derived alcohol" . | JOURNAL OF MATERIALS CHEMISTRY A 12 . 30 (2024) : 19029-19038 . |
| APA | Zhang, Lin-Xing , Tang, Zi-Rong , Qi, Ming-Yu , Xu, Yi-Jun . Engineering semiconductor quantum dots for co-upcycling of CO2 and biomass-derived alcohol . | JOURNAL OF MATERIALS CHEMISTRY A , 2024 , 12 (30) , 19029-19038 . |
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Photo-driven cross-coupling of o-arylenediamines and alcohols has emerged as an alternative for the synthesis of bio-active benzimidazoles. However, tackling the key problem related to efficient adsorption and activation of both coupling partners over photocatalysts towards activity enhancement remains a challenge. Here, we demonstrate an efficient interface synergy strategy by coupling exposed oxygen vacancies (VO) and Pd Lewis acid sites for benzimidazole and hydrogen (H2) coproduction over Pd-loaded TiO2 nanospheres with the highest photoredox activity compared to previous works so far. The results show that the introduction of VO optimizes the energy band structure and supplies coordinatively unsaturated sites for adsorbing and activating ethanol molecules, affording acetaldehyde active intermediates. Pd acts as a Lewis acid site, enhancing the adsorption of alkaline amine molecules via Lewis acid-base pair interactions and driving the condensation process. Furthermore, VO and Pd synergistically promote interfacial charge transfer and separation. This work offers new insightful guidance for the rational design of semiconductor-based photocatalysts with interface synergy at the molecular level towards the high-performance coproduction of renewable fuels and value-added feedstocks. We propose a highly efficient interface synergy strategy that integrates exposed VO sites with surface Pd Lewis acid sites to ensure effective adsorption and activation of both coupling partners, o-arylenediamines and alcohols, with the synergistic interaction between VO and Pd enhancing interfacial charge transfer, thereby achieving the highest performance so far in the field of photoredox mediated benzimidazole synthesis. image
Keyword ：
benzimidazoles synthesis benzimidazoles synthesis defect defect hydrogen evolution hydrogen evolution interface synergy interface synergy photoredox catalysis photoredox catalysis
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| GB/T 7714 | Huang, Zhi-Sang , Wang, Yin-Feng , Qi, Ming-Yu et al. Interface Synergy of Exposed Oxygen Vacancy and Pd Lewis Acid Sites Enabling Superior Cooperative Photoredox Synthesis [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (47) . |
| MLA | Huang, Zhi-Sang et al. "Interface Synergy of Exposed Oxygen Vacancy and Pd Lewis Acid Sites Enabling Superior Cooperative Photoredox Synthesis" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 47 (2024) . |
| APA | Huang, Zhi-Sang , Wang, Yin-Feng , Qi, Ming-Yu , Conte, Marco , Tang, Zi-Rong , Xu, Yi-Jun . Interface Synergy of Exposed Oxygen Vacancy and Pd Lewis Acid Sites Enabling Superior Cooperative Photoredox Synthesis . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (47) . |
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The scarcity of strategies to finely modulate the interface assembly between MXene and semiconductors often restricts their full potential for photocatalysis. Herein, resorting to the cetyltrimethylammonium bromide (CTAB) surfactant intercalation effect, we report the rational synthesis of hierarchical seaurchin-like CdS-Ti3C2T x MXene-CTAB (CdS-T-C) ensembles to modulate the interface and structure of MXene-semiconductor heterojunctions for significantly boosted photoredox coupling catalysis. The ternary CdS-T-C exhibits markedly enhanced activity toward visible light photoreforming of benzyl alcohol (BA) to benzaldehyde (BAD) and H2 cooperatively, as compared to bare CdS and conventional CdS-Ti3C2T x MXene (CdS-T) that suffer from serious MXene restacking with obvious electronic and optical property attenuation. Mechanistic studies reveal that the CTAB interfacial intercalation alleviates the restacking of Ti3C2T x , thus weakening the light shielding effect while promoting the charge transport and surface activity of MXene. This work demonstrates an appealing strategy to regulate the interfacial cross-coupling configuration of MXene-semiconductor composites for efficient solar-to-chemical conversion.
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| GB/T 7714 | Zhang, Hanbo , Si, Tingting , Yuan, Lan et al. Surfactant-Assisted Assembly of Hierarchical CdS-Ti3C2T x MXene toward Enhanced Cooperative Photoredox Catalysis [J]. | ACS MATERIALS LETTERS , 2024 , 7 (1) : 257-264 . |
| MLA | Zhang, Hanbo et al. "Surfactant-Assisted Assembly of Hierarchical CdS-Ti3C2T x MXene toward Enhanced Cooperative Photoredox Catalysis" . | ACS MATERIALS LETTERS 7 . 1 (2024) : 257-264 . |
| APA | Zhang, Hanbo , Si, Tingting , Yuan, Lan , Han, Chuang , Xu, Yi-Jun . Surfactant-Assisted Assembly of Hierarchical CdS-Ti3C2T x MXene toward Enhanced Cooperative Photoredox Catalysis . | ACS MATERIALS LETTERS , 2024 , 7 (1) , 257-264 . |
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