查看更多>>摘要：Electrochemical hydrogen evolution reaction (HER) coupled with microplastics reforming are critical for marine energy and environmental engineering, but filled with challenges. Herein, Ni3N/W5N4 Janus nanostructure with barrier-free heterointerface was designed via transition metal nitrides-inducing growth strategy. Benefiting from the interface synergistic effect, super-hydrophilic surface and multilevel Janus structure, Ni3N/W5N4 electrode displays Pt-like HER performance and the outstanding stability (similar to 300 h) under industrially current. Meanwhile, Ni3N/W5N4 also exhibits high activity and selectivity toward electro-reforming of plastics, showing an ultralow overpotential of 1.33 V (eta(10)) and generating the value-added HCOOH with the high Faradic efficiency of-85%. Impressively, driven by solar panels, the bifunctional Ni3N/W5N4 electrocatalyst achieves the highly efficient production of H-2 and HCOOH (eta(10) =1.4 V-eta solar to hydrogen=16.04%) in seawater full of plastics. This work underlines the on-site upgrading of plastic wastes and energy-saving hydrogen evolution in seawater enabled by the design of Janus heterostructures for metal nitrides.
查看更多>>摘要：In this study, a general strategy is demonstrated to prepare a partially oxidized three-dimensional (3D) porous ruthenium (Ru) aerogel with distinct porous architecture and unique Ru/RuO2 interface. The optimized partially oxidized Ru aerogel catalyst exhibits an exceptional HER performance, which is even superior to the benchmark Pt/C catalyst, and an outstanding OER efficiency that is better than commercial RuO2 in both alkaline and acidic solutions. Furthermore, a two-electrode configuration based on the partially oxidized Ru aerogel as both anode and cathode for the overall water splitting exhibits an ultra-low working voltage of 1.467 V in 1 M KOH and 1.468 V in 0.5 M H2SO4 at 10 mA cm(-2) as well as a satisfactory long-term stability, outperforming the device composed of Pt/C||RuO2 catalysts. This research opens up a new avenue to develop highly efficient 3D porous aerogel electrocatalysts toward overall water splitting applications.
查看更多>>摘要：Significant health risk exists due to increasing antibiotic-resistant bacteria and formation of antibiotic-resistant bacterial biofilm in water. For comprehensive understanding of stress response mechanisms of biofilm formation under sub-lethal photocatalysis (PC), Herein, a drip flow device was developed to culture biofilm and Pseudomonas aeruginosa (GEN) (resistance to Gentamicin) was developed to assess the effect of sub-lethal PC on biofilm formation. Under sub-lethal PC, the bacterial abundance and the thickness of biofilm decreased relative to controls (by 81.7% and 68.0%, respectively) on the 1st day; however, the content of extracellular polymeric substance (EPS) per cell was promoted unexpectedly. Furthermore, it was found that the proportion of viable culturable bacteria in the biofilm increased 7.8 times relative to control and the biofilm exhibited resistance to oxidative stress via EPS secretion. This perspective was validated through molecular regulatory network study. This study may provide enlightenment to bacterial biofilm control in the water system.
查看更多>>摘要：Ni doping is an effective way to change the electronic structure of molybdenum carbide (Mo2C) to promote the hydrogen evolution reaction (HER) performance. However, the relationship between the Ni dopant concentration and HER activity remains to be explored. Herein, we prepare self-sanding Mo2C electrodes with different Ni concentrations, and employ density functional theory (DFT) calculations along with electrochemical tests to investigate the effect of the Ni dopant concentration on HER activity. The Mo and C come from the co-deposition of MoO(4)(2-)and CO(3)(2-)on a Ni substrate that supplies Ni dopant. The concentration of Ni dopant can be tuned by adjusting the temperature. The HER performance of the Mo2C electrodes with various Ni dopant concentrations is in line with DFT calculations that the optimized Ni-Mo2C-0.67 electrode has a lowest delta G(H*) value of -0.13 eV. Altogether, this work sheds light on controllably designing Ni-doped Mo2C electrodes for splitting water.
查看更多>>摘要：Embedding Ni nanoparticles (NPs) into supports has been widely accepted as one of solutions for Ni confinement, but high loading usually stands on the opposite of being well dispersed and encapsulated. Herein, we developed a controlled 'dissolution-recrystallization' method of embedding high loading and uniform Ni NPs into the shell of hollow silicalite-1 (S-1) zeolite. The sizes of Ni NPs maintained at ca. 4-5 nm with increasing Ni loading from 3% to 20%, and the TOF kept at ca. 60 s(-1) (800 ?) in the dry reforming of methane reaction. The augmented density of active sites with Ni loading rendered an outstanding reaction rate of 20.0 molCH(4)/g(cat)/h over 20% Ni@S-1. The embedded structure also endowed a good stability upon running for 150 h. This study paves the way for embedding high loading and uniform metal nanoparticles inside the zeolite, providing an effective strategy to stabilize metals under harsh reaction conditions.
查看更多>>摘要：Light-driven thermocatalysis has emerged as an attractive approach for catalytic oxidation of volatile organic compounds (VOCs). Herein, we have synthesized Pt-mTiO(2)/USY nanocomposites for the catalytic degradation of toluene under full solar spectrum. The mTiO(2)/USY with increasing Pt content show increased activity, among which 0.9Pt-mTiO(2) exhibits toluene conversion of 86.6% and CO2 yield of 74.5% at 243 degrees C with a light intensity of 490 mW/cm(2) under 5 vol.% water vapor. The high catalytic performance of Pt-mTiO(2)/USY can be attributed to the large surface area, strong light absorption, highly efficient conversion of light-to-heat, abundant oxygen vacancies, uniform Pt distribution, and Ti3+ species on the catalyst surface. The introduction of Pt nanoparticles (NPs) in mTiO(2)/USY enhances light absorption and improves the mobility of surface lattice oxygen. The combination of EPR, O-2-TPD, and in situ DRIFTS analysis reveals that light irradiation further stimulates more active lattice oxygen to participate in the toluene oxidation.
Li, ChuangJang, HaeseongKim, Min GyuHou, Liqiang...
8页
查看更多>>摘要：Designing highly efficient Pt-free electrocatalysts with low overpotential for the alkaline hydrogen evolution reaction (HER) remains a significant challenge. In this paper, we successfully construct Ru-incorporated oxygen-vacancy-enriched MoO2 nanosheets (Ru/MoO2_x) for the HER through a "one stone two birds " strategy. This strategy can solve two urgent problems simultaneously, the intrinsic electrochemical activity of original MoO(2 )is far from satisfactory and the H2O adsorption/dissociation abilities of Ru are weak. Specifically, the oxygen-vacancy-enriched MoO3 serves as an excellent platform for anchoring and trapping Ru ions. In-depth analyses indicate that the incorporation of Ru nanoclusters induces transition from MoO3 to MoO2, generates oxygen vacancies, and creates Ru-O-Mo sites. The synergistic effect of Ru nanoclusters, Ru-O-Mo sites and oxygen-vacancy-enriched MoO2 will endow the obtained catalyst excellent electrocatalytic activity. In particular, the optimal Ru/MoO2_x electrocatalyst delivered a low overpotential of 29 mV at 10 mA cm(_2) in a basic electrolyte.
查看更多>>摘要：The intensification of electron transport between the dual-reaction centres in Fenton-like catalyst is demonstrated through the incorporation of carbon-metal (C-M) bond bridges. Herein, nitrogen-doped carbon nanotubeencapsulated Fe3C (Fe3C@NCNT) with dual-reaction centres over short C-Fe bond was constructed through DFT calculation, and accordingly a series of NCNTs-encapsulated Fe/Fe3C, Co, and Mo2C nanoparticles on carbonised loofah were developed by dynamic thermal impregnation and subsequent pyrolysis process. The resultant catalysts displayed satisfactory degradation properties of antibiotics, in which Fe/Fe3C@NCNTs-CL-800 achieved norfloxacin (NOR) removal efficiency of 93.8% in 90 min under neutral pH, and presented excellent cycle stability in NOR removal as well as universality in various antibiotic degradation systems. The remarkable degradation performance of heterogeneous Fenton-like catalysts was attributed to enhancing electron transport to electron-rich M centres over short C-M bond bridges. This study will open a new perspective on the rational design of catalysts for Fenton-like degradation.
查看更多>>摘要：Tungsten-based catalyst has been widely investigated in the field of selective hydrogenolysis of secondary C-O bond, such an important yet challenging strategy, in glycerol conversion, in which the product 1,3-propanediol (1,3-PDO) is of great value in polyester industry. Unfortunately, though it has been proved to be highly active, the identification of the intrinsic tungsten oxide active sites still remains unrevealed to date due to its complex microstructure. Herein, we incorporate atomically dispersed alumina as promoter in the context of the selective hydrogenation of glycerol and report a Pt/Al-WOx catalyst. This catalyst decidedly outperforms the unpromoted Pt/WOx, which elevates the 1,3-PDO yield to 2 times. Spectroscopy characterizations and chemisorption experiments have revealed that the high activity and selectivity of Pt/Al-WO(x & nbsp;)catalyst results from the more oxygen vacancies on WOx in-situ generation by the acceleration of atomically dispersed alumina in hydrogen atmosphere, which increases the selective adsorption of glycerol and the in-situ Bronsted acid sites for the selective activation of secondary C-O bonds, thus largely augmenting the hydrogenolysis performance. This discovery not only provides the new strategy of defect engineering to enhance hydrogenolysis performance of secondary C-O bond in biomass compounds, but reveals the unique role of the unsaturated coordination structure of WOx in chemoselective hydrogenolysis reactions.
查看更多>>摘要：Photothermocatalysis is usually the photoinduced thermal effect to drive the catalytic reaction assisted by high oxidizing radials from photocatalysis. Herein, a carbon nitride-induced urchin-like catalyst Co3O4-CoO-CN (abbreviated as CoOx-CN) with abundant peripheral branches is synthesized through the solvothermal reaction and calcination at different temperatures. An appropriate calcination temperature can remove partial CN structure and help to promote the light absorption, maintain the high specific surface area, and produce enough active oxygen species and active sites. CoOx-CN-300 exhibits the good catalytic activity with toluene conversion of 83.8% and CO2 yield of 79.6% under the full spectrum irradiation, where photocatalysis plays an important role in igniting catalytic reaction and light-to-thermal conversion provides high temperature to fulfil intermediates mineralization. Furthermore, light irradiation can enhance the light-driven thermocatalytic performance of CoOx-CN-300 compared to conventional thermocatalytic activity by activating more lattice oxygen and inducing the formation of more oxygen vacancies to participate in the oxidation reaction.
NSTL
Elsevier