| 1. |
- Cai, Bin, et al.
(författare)
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Organic Polymer Dots Photocatalyze CO2 Reduction in Aqueous Solution
- 2023
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Ingår i: Angewandte Chemie International Edition. - : John Wiley & Sons. - 1433-7851 .- 1521-3773. ; 62:45
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Tidskriftsartikel (refereegranskat)abstract
- Developing low-cost and efficient photocatalysts to convert CO2 into valuable fuels is desirable to realize a carbon-neutral society. In this work, we report that polymer dots (Pdots) of poly[(9,9 ' -dioctylfluorenyl-2,7-diyl)-co-(1,4-benzo-thiadiazole)] (PFBT), without adding any extra co-catalyst, can photocatalyze reduction of CO2 into CO in aqueous solution, rendering a CO production rate of 57 mu mol g(-1) h(-1 )with a detectable selectivity of up to 100 %. After 5 cycles of CO2 re-purging experiments, no distinct decline in CO amount and reaction rate was observed, indicating the promising photocatalytic stability of PFBT Pdots in the photocatalytic CO2 reduction reaction. A mechanistic study reveals that photoexcited PFBT Pdots are reduced by sacrificial donor first, then the reduced PFBT Pdots can bind CO(2 )and reduce it into CO via their intrinsic active sites. This work highlights the application of organic Pdots for CO2 reduction in aqueous solution, which therefore provides a strategy to develop highly efficient and environmentally friendly nanoparticulate photocatalysts for CO2 reduction.
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| 2. |
- Cheng, Fangwen, et al.
(författare)
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Interfacial Property Tuning Enables Copper Electrodes in High-Performance n-i-p Perovskite Solar Cells
- 2023
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 145:36, s. 20081-20087
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Tidskriftsartikel (refereegranskat)abstract
- Developing cost-effective metal electrodes is essential for reducing the overall cost of perovskite solar cells (PSCs). Although copper is highly conductive and economical, it is rarely used as a positive electrode in efficient n-i-p PSCs due to its unmatched Fermi level and low oxidation threshold. We report herein that modification for the inner surface of electrodes using mercaptopyridine-based molecules readily tunes the electronic and chemical properties of copper, which has been achieved by fine-tuning the substituents of mercaptopyridines. The systematic adjustment for the Fermi level and oxidation potential of copper facilitates interfacial hole extraction and enhances the oxidation resistance of copper electrodes, which enables pure copper electrodes to be used in high-performance n-i-p PSCs with different hole transport materials. The resulting PSCs with copper electrodes display excellent power conversion efficiency and long-term stability, even comparable to those of the gold electrodes, showing great potential in the manufacturing and commercialization of PSCs.
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| 3. |
- Huang, Xiaofeng, et al.
(författare)
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Solvent racing crystallization : Low-solvation dispersion cosolvents for high-quality halide perovskites in photovoltaics
- 2023
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Ingår i: Joule. - : Elsevier. - 2542-4351. ; 7:7, s. 1556-1573
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Tidskriftsartikel (refereegranskat)abstract
- The solvation capacity of dispersion solvents plays a crucial role in the solution processing of metal halide perovskites. For instance, N,N-dimethylformamide (DMF), a widely used dispersion solvent, possesses high solvation capacity but often generates suboptimal film quality due to slow crystallization kinetics. We propose using low-solvation binary cosolvents (nitrile-and ether-type solvents) to achieve a balance between solvation (i.e., sufficient solubility of precursors) and desolvation (i.e., rapid crystallization of films) pro-cesses during perovskite synthesis. The polarity and hydrogen -bonding property of these cosolvents synergistically enhance their solvation capacity, facilitating perovskite precursor dissolution. Moreover, the low-solvation cosolvents accelerate the crystalliza-tion of well-defined intermediate films, yielding higher-quality pe-rovskites than those synthesized with DMF. The optimized modules achieved an active-area efficiency of 22.27%, with a certified aper-ture-area efficiency of 16.10% and corresponding active-area effi-ciency of 20.75%. This research on solvation regulation provides universal guidelines for innovatively preparing high-quality halide perovskites.
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| 4. |
- Liu, Tianqi, et al.
(författare)
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Bioinspired Active Site with a Coordination-Adaptive Organosulfonate Ligand for Catalytic Water Oxidation at Neutral pH
- 2023
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 145:21, s. 11818-11828
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Tidskriftsartikel (refereegranskat)abstract
- Many enzymes use adaptive frameworks to preorganize substrates, accommodate various structural and electronic demands of intermediates, and accelerate related catalysis. Inspired by biological systems, a Ru-based molecular water oxidation catalyst containing a configurationally labile ligand [2,2′:6′,2″-terpyridine]-6,6″-disulfonate was designed to mimic enzymatic framework, in which the sulfonate coordination is highly flexible and functions as both an electron donor to stabilize high-valent Ru and a proton acceptor to accelerate water dissociation, thus boosting the catalytic water oxidation performance thermodynamically and kinetically. The combination of single-crystal X-ray analysis, various temperature NMR, electrochemical techniques, and DFT calculations was utilized to investigate the fundamental role of the self-adaptive ligand, demonstrating that the on-demand configurational changes give rise to fast catalytic kinetics with a turnover frequency (TOF) over 2000 s–1, which is compared to oxygen-evolving complex (OEC) in natural photosynthesis.
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| 5. |
- Zhang, Wuyong, et al.
(författare)
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Coordinative Stabilization of Single Bismuth Sites in a Carbon-Nitrogen Matrix to Generate Atom-Efficient Catalysts for Electrochemical Nitrate Reduction to Ammonia
- 2023
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Ingår i: Advanced Science. - : John Wiley & Sons. - 2198-3844. ; 10:28
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Tidskriftsartikel (refereegranskat)abstract
- Electrochemical nitrate reduction to ammonia powered by renewable electricity is not only a promising alternative to the established energy-intense and non-ecofriendly Haber-Bosch reaction for ammonia generation but also a future contributor to the ever-more important denitrification schemes. Nevertheless, this reaction is still impeded by the lack of understanding for the underlying reaction mechanism on the molecular scale which is necessary for the rational design of active, selective, and stable electrocatalysts. Herein, a novel single-site bismuth catalyst (Bi-N-C) for nitrate electroreduction is reported to produce ammonia with maximum Faradaic efficiency of 88.7% and at a high rate of 1.38 mg h(-1) mg(cat)(-1) at -0.35 V versus reversible hydrogen electrode (RHE). The active center (described as BiN2C2) is uncovered by detailed structural analysis. Coupled density functional theory calculations are applied to analyze the reaction mechanism and potential rate-limiting steps for nitrate reduction based on the BiN2C2 model. The findings highlight the importance of model catalysts to utilize the potential of nitrate reduction as a new-generation nitrogen-management technology based on the construction of efficient active sites.
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| 6. |
- Zhang, Yazhou, et al.
(författare)
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Heterogeneous Hydrogenation with Hydrogen Spillover Enabled by Nitrogen Vacancies on Boron Nitride-Supported Pd Nanoparticles
- 2023
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Ingår i: Angewandte Chemie International Edition. - : Wiley-VCH Verlagsgesellschaft. - 1433-7851 .- 1521-3773. ; 62:9
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Tidskriftsartikel (refereegranskat)abstract
- Heterogeneous hydrogenation with hydrogen spillover has been demonstrated as an effective route to achieve high selectivity towards target products. More effort should be paid to understand the complicated correlation between the nature of supports and hydrogenation involving hydrogen spillover. Herein, we report the development of the hydrogenation system of hexagonal boron nitride (h-BN)-supported Pd nanoparticles for the hydrogenation of aldehydes/ketones to alcohols with hydrogen spillover. Nitrogen vacancies in h-BN determine the feasibility of hydrogen spillover from Pd to h-BN. The hydrogenation of aldehydes/ketones with hydrogen spillover from Pd proceeds on nitrogen vacancies on h-BN. The weak adsorption of alcohols to h-BN inhibits the deep hydrogenation of aldehydes/ketones, thus leading to high catalytic selectivity to alcohols. Moreover, the hydrogen spillover-based hydrogenation mechanism makes the catalyst system exhibit a high tolerance to CO poisoning.
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| 7. |
- Zhang, Zhicheng, et al.
(författare)
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The Editorial
- 2023
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Ingår i: Chemistry - An Asian Journal. - : John Wiley & Sons. - 1861-4728 .- 1861-471X. ; 18:6
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Tidskriftsartikel (övrigt vetenskapligt/konstnärligt)abstract
- Surface and interface engineering has been considered as a promising strategy to enhance the performance of catalysts towards CO2 reduction. In their editorial to this special collection, guest editors Zhicheng Zhang, Zhen Zhang, Zhenyu Sun, Shaoqi Zhan and Guoxiong Wang provide a brief overview of this field and highlight the state-of-the-art contributions featured in this special collection.
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| 8. |
- Zhou, Yue, et al.
(författare)
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Stabilized and Controlled Release of Radicals within Copper Formate-Based Nanozymes for Biosensing
- 2023
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 15:37, s. 43431-43440
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Tidskriftsartikel (refereegranskat)abstract
- Fenton-like radical processes are widely utilized to explain catalytic mechanisms of peroxidase-like nanozymes, which exhibit remarkable catalytic activity, cost-effectiveness, and stability. However, there is still a need for a comprehensive understanding of the formation, stabilization, and transformation of such radicals. Herein, a copper formate-based nanozyme (Cuf-TMB) was fabricated via a pre-catalytic strategy under ambient conditions. The as-prepared nanozyme shows comparable catalytic activity (K-m, 1.02 x 10(-5) mM(-1); K-cat, 3.09 x 10(-2) s(-1)) and kinetics to those of natural peroxidase toward H2O2 decomposition. This is attributed to the feasible oxidation by *OH species via the *O intermediate, as indicated by density functional theory calculations. The key .OH radicals were detected to be stable for over 52 days and can be released in a controlled manner during the catalytic process via in situ electron spin-resonance spectroscopy measurements. Based on the understanding, an ultrasensitive biosensing platform was constructed for the sensitive monitoring of biochemical indicators in clinic settings.
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