查看更多>>摘要：? 2021 Elsevier B.V.The authors regret that Figs. 1 and 2b have been published erroneously. Therefore, the authors would like to replace it with the correct one given below. In current version, the mean particle size of prepared nanoparticle is about 3.94 nm as shown in TEM image. This does not alter the discussion. The authors confirm that this change does not affect the originality and importance of the scientific findings reported in the paper. The authors would like to apologise for any inconvenience caused. [Figure presented] Fig. 1. TEM image (a), HRTEM image (b) and the particle size histogram (d) of Pt@GO-PVP NPs. [Figure presented] Fig. 2. (b) Raman spectra of GO and Pt@GO-PVP.
查看更多>>摘要：? 2021 Elsevier B.V.The authors regret that Figure 1 and 2 have been published erroneously. Therefore, the authors would like to replace it with the correct one given below. In current version, the mean particle size of prepared nanoparticle is about 4.19 nm as shown in TEM image. This does not alter the discussion. The authors confirm that this change does not affect the originality and importance of the scientific findings reported in the paper. The authors would like to apologise for any inconvenience caused. [Figure presented] Fig. 1. (b) Raman spectra of GO and TC@GO [Figure presented] Fig. 2. (a) TEM image, (b) particle size histogram RhPt/TC@GO NPs.
查看更多>>摘要：? 2022 Elsevier B.V.The rational design of the highly active, durable, and cost-effective catalysts for oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER) is essential for next-generation water splitting systems and zinc-air batteries. Herein, a novel strategy is demonstrated to design iron tin oxyselenide (FexSn1?xOSe) with enriched oxygen vacancies through a simple and straightforward hydrothermal and subsequent selenization process. The optimal Fe0.33Sn0.67OSe catalyst exhibits superior ORR, OER, and HER performances due to the numerous electroactive sites and high synergistic effects. The water electrolyzer requires a small voltage of 1.490 V and incredible reversibility over 24 h. Most interestingly, the Fe0.33Sn0.67OSe air-cathode based flexible ZAB exhibits a high power density of 153.96 mW cm?2 and ultralong cycle life for 400 h. This work opens a new strategy to establish highly active and durable multifunctional catalysts in next-generation energy conversion and storage systems.
查看更多>>摘要：? 2021Defect engineering, inducing photo-excited electrons and holes to different surfaces of semiconductor photocatalyst, is an efficient strategy to improve the photocatalytic activity. A rapid heating-up hydrothermal technique is developed to regulate ZnIn2S4 crystal growth, then, ultrathin ZnIn2S4 nanosheets with In defect-rich [InS]6 interlayer but perfect [InS]4 and [ZnS]4 surface layers are successfully prepared (ultra-ZIS-VIn). Interestingly, the In defect, inducing the redistribution of the orbitals near the valence band maximum, separates the oxidation and reduction sites on the opposite sides of the ultra-ZIS-VIn nanosheets. Simultaneously, In defects increase the density of states (near the valence band maximum and conduction band minimum) and delocalize the electron around In defects. Accordingly, the photocatalytic hydrogen evolution rate is optimized to 13.4 mmol h?1 g?1, which is 8.9 times higher than that of defect-free ZnIn2S4 (pristine-ZIS).
查看更多>>摘要：? 2021 Elsevier B.V.The application of hematite(α-Fe2O3)-based photoanodes in photoelectrochemical (PEC) water oxidation has been hampered by disgusting charge recombination and difficult carrier migration. Herein, we modified indium sulfide (In2S3) nanoparticles on the surface of fluorine-doped α-Fe2O3 (F-Fe2O3) nanorods. The In2S3/F-Fe2O3 heterostructure bonded by S-O chemical bond shows a superior photocurrent density of 2.21 mA cm?2 at 1.23 V versus reversible hydrogen electrode (around 3.45 times higher than that of pristine α-Fe2O3). In-depth investigations show that In2S3/F-Fe2O3 has significantly increased donor density and decreased charge transfer resistance. Simultaneously, In2S3 decorated with S-O bond could reduce the surface defect states. Further studies of energy band location reveal the formation of type-Ⅱ heterojunction between In2S3 and F-Fe2O3. The unique heterostructure provides a powerful driving force for charge separation and transport, resulting in satisfactory bulk phase and surface separation efficiency. This work provides ideas for the design and study of multicomponent photoanodes.
查看更多>>摘要：? 2021 Elsevier B.V.This study investigated the Cu-CeO2 interactions for CO hydrogenation to methanol by applying rate measurements, chemical titration/desorption, together with in-situ/operando spectroscopy techniques under realistic reaction conditions. Ce components were enriched in the surface region of Cu/CeO2 catalysts while Ce3+ and Ce4+ atoms co-existed during CO hydrogenation. The ratio of Ce3+ to Cu0 in the surface region of catalysts increased linearly with the Ce content. The turnover rates of CH3OH formation increased as a single-valued function of the ratio, irrespective to the individual contact extent between Cu and CeO2 clusters or Ce content in the Cu/CeO2 catalysts, indicating that the Cu0-Ce3+ sites pair acts as active sites for CO hydrogenation to methanol over Ce-CeO2 samples. This study also unraveled that formyl and formate species, as reactive surface intermediates, were co-adsorbed on the Cu0-Ce3+ sites, and their hydrogenation routes occurred concurrently for CH3OH formation during CO-H2 reactions.
查看更多>>摘要：? 2021 Elsevier B.V.In this work, we first applied metal-free polymeric catalysts to drive the photocatalytic denitrification (PCDN) reaction under visible light. We developed a hydrothermal-transverse thermal stripping method to prepare Cl/S co-doped metal-free carbon nitride nanotubes as the photocatalysts (Cl/S-TCN). With larger specific surface area, stronger light response intensity and wider light absorption range, the PCDN performance of Cl/S-TCN was 19 times higher than that of carbon nitride (GCN, obtained by direct calcination of melamine) under visible light. In hole scavenger experiments, the PCDN reaction was dominated by photo-generated electrons (e-) over Cl/S-TCN in acidic solutions. DFT calculations showed that surface Cl and S dopants preferentially adsorbed the O atoms in NO3- and delivered photoinduced-e- to N atoms through O atoms, ultimately breaking the N-O bond. Such reaction pathway was rarely reported in previous studies. Hence, this work contributes to the first insight into PCDN catalyzed by atomically modified metal-free photocatalyst under visible light.
查看更多>>摘要：? 2021Herein, a multi-shelled hollow micro-reactor with tunable shell number, thickness and porosity is constructed by nanosized Co3O4 to catalyze peroxymonosulfate (PMS) for the first time. Triple-shelled hollow microspheres (TS-HM) exhibit superior catalytic activity with the degradation rate of 0.4158 min?1, which is 22, 5.8, 1.9 times of that of solid nanoparticles, quadruple-shelled hollow microspheres (QS-HM), and double-shelled hollow microspheres (DS-HM), respectively. Such an outstanding performance of TS-HM is attributed to more exposed active sites, strong capacity of CoII regeneration and desired structure stability. Furthermore, the selectivity of 2-cholorophenol (2-CP) over humic acid (HA) is optimized by tuning shell thickness and porosity. The thick shell and narrow pore size are recognized as the dominant contributors based on size exclusion effects. Significantly, mechanistic studies reveal that O2·? is generated on the catalyst surface via O2 adsorption and reduction by oxygen vacancies, and plays an important role for CoII regeneration.
查看更多>>摘要：? 2021The strong metal-support interaction (SMSI) effect is attractive for improving the activity and durability of metal catalyst. Here, we uncovered that the strong polar bond in support can significantly boost the electrocatalytic oxygen reduction activity and durability of Pd nanoparticles (NPs). The mass-specific activity and surface-specific activity of optimized Pd/p-BNO at 0.90 V (vs.RHE) is almost 1.9 and 2.2 times higher than that of commercial Pt/C catalyst, respectively. By means of a joint experimental and computational study, the enhanced activity of Pd/p-BNO stems from the electron directly transfer through the strong polar O–B bonds from support to Pd NPs leading to the electron-rich Pd surface. Moreover, the strong bonding effect of the caused by polarity bond effectively improves the stability of Pd/p-BNO. This progress demonstrates the vital role of polar chemical bonds in support on inducing SMSI effect, which might open up new opportunities in designing superior heterogeneous catalysts.
查看更多>>摘要：? 2021 Elsevier B.V.Electrochemical nitrate reduction (NO3-RR) to synthesize ammonia is considered to be a promising strategy to enable artificial nitrogen cycle. Great efforts have been devoted to improving the efficiency and selectivity of the electrocatalysts for NO3-RR. Herein, we demonstrate that tuning the oxygen chemical environment via Ar plasma treatment is an effective approach to improve the NO3-RR activity of Cu2O. Combining synchrotron-based X-ray absorption spectroscopy and other advanced spectroscopy techniques, we find that plasma treatment can effectively promote the formation of oxygen vacancies and hydroxyl groups on Cu2O surface. In-situ diffuse-reflectance infrared Fourier transform spectroscopy and density functional theory calculation further reveal that oxygen vacancies and hydroxyl groups facilitate the adsorption of nitrate and proton transfer on the Cu2O surface, thus leading to improved ammonia selectivity. Our results clarify the critical role of surface oxygen species for NO3-RR and can guide the design of other electrocatalysts via surface engineering.
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