Construction of Dual-Active Sites by Interfacing with Polyhydroxy Fullerene on Nickel Hydroxide Surfaces to Promote CO2 Deep Photoreduction to CH4.

Due to the complex series of elementary steps involved, achieving deep photoreduction of CO2 to multielectron products such as CH4 remains a challenging task. Therefore, it is crucial to strategically design catalysts that facilitate the controlled formation of the crucial intermediates and provide precise control over the reaction pathway. Herein, we present a pioneering approach by employing polyhydroxy fullerene (PHF) molecules to modify the surface of Ni(OH)2, creating stable and effective synergistic sites to enhance the formation of CH4 from CO2 under light irradiation. As a result, the optimized PHF-modified Ni(OH)2 cocatalyst achieves a CH4 production rate of 455 µmol g-1 h-1, with an electron-based selectivity of approximately 60%. The combination of in situ characterizations and theoretical calculations reveals that the hydroxyl species on the surface of PHF can participate in stabilizing crucial intermediates and facilitating water activation, thereby altering the reaction pathway to form CH4 instead of CO. This study provides a novel approach to regulating the selectivity of photocatalytic CO2 reduction by exploring molecular surface modification through interfacing with functionalized carbon clusters.

Self-standing three-dimensional PdAu nanoflowers for plasma-enhanced photo-electrocatalytic methanol oxidation with a CO-free dominant mechanism.

Precise design of high efficacious catalysts and the insight into the mechanism for photo-electrocoupling catalytic methanol oxidation reaction (MOR) are two major issues for the development and practical application of direct methanol fuel cells (DMFCs). Herein, a novel self-standing three-dimensional nanosheet assembly PdAu nanoflower with local surface plasmon resonance effect is fabricated to acquire excellent catalytic performance and explore the photo-electrocatalytic mechanism for MOR. Interestingly, the Pd1Au1 nanoflower electrocatalyst exhibits superior mass activity than pure Pd and Pd/C catalysts thanks to the abundant active sites and efficacious charge transfer. Further on, with the assistance of LSPR effect, the catalytic activity for MOR of Pd1Au1 catalyst (4179.04 mA mg-1Pd) under visible light illumination achieved 2.41-fold than dark conditions (1731.42 mA mg-1Pd). Moreover, the long-term durability of Pd1Au1 catalysts with visible light is also improved compare to dark condition and other mentioned Pd catalyst. More significantly, a photo-electrocoupling CO-free dominant mechanism is proposed to in-depth understand the promotion of catalytic activity and durability for MOR. This contribution provides the rational design of plasma-enhanced high-effective photo-electrocatalyst and reveals a CO-free dominant MOR mechanism for the progress of future liquid direct fuel cells.

Observed inequality in urban greenspace exposure in China.

Given the important role of green environments playing in healthy cities, the inequality in urban greenspace exposure has aroused growing attentions. However, few comparative studies are available to quantify this phenomenon for cities with different population sizes across a country, especially for those in the developing world. Besides, commonly used inequality measures are always hindered by the conceptual simplification without accounting for human mobility in greenspace exposure assessments. To fill this knowledge gap, we leverage multi-source geospatial big data and a modified assessment framework to evaluate the inequality in urban greenspace exposure for 303 cities in China. Our findings reveal that the majority of Chinese cities are facing high inequality in greenspace exposure, with 207 cities having a Gini index larger than 0.6. Driven by the spatiotemporal variability of human distribution, the magnitude of inequality varies over different times of the day. We also find that exposure inequality is correlated with low greenspace provision with a statistical significance (p-value < 0.05). The inadequate provision may result from various factors, such as dry cold climate and urbanization patterns. Our study provides evidence and insights for central and local governments in China to implement more effective and sustainable greening programs adjusted to different local circumstances and incorporate the public participatory engagement to achieve a real balance between greenspace supply and demand for developing healthy cities.

Enhancement of the activity of Cu/TiO2 catalyst by Eu modification for selective catalytic reduction of NOx with NH3.

The Cu/TiO2 catalysts with the addition of Eu were developed by the sol-gel way for the selective catalytic reduction (SCR) of NOx by NH3. Activity tests revealed that CuEu/TiO2-0.15 catalyst showed the optimal de-NOx performance in a wide temperature range (150-300 °C), along with an admirable SO2 tolerance. According to characterization analysis, the relationship between the NH3-SCR performance and physicochemical characters of samples was explored. The adjunction of Eu on Cu/TiO2 catalyst can contribute to the formation of a large amount of Cu2+, adsorbed oxygen, and acid sites on the catalyst surface. Moreover, the Eu addition on Cu/TiO2 is favorable to the generation of activated NOx and NH3 substances adsorbed on the catalyst surface, which would conduce to the NH3-SCR process by Langmuir-Hinshelwood (L-H) mechanism effectively.

Experimental Investigation of the Fluidization Reduction Characteristics of Iron Particles Coated with Carbon Powder under Pressurized Conditions.

The purpose of this study was to comprehensively analyze the effects of the carbon powder coating mass fraction, pressure, reduction temperature, reduction time, gas linear velocity, and particle size on fluidization reduction. Brazilian fine iron ore particles were the experimental object, and reduction experiments were performed under added carbon powder coating and pressure conditions. A six-factor, three-level orthogonal experiment method was used to obtain the optimal operating conditions and investigate the adhesion and inhibition mechanisms of fine iron ore during reduction. The experimental results show that with the addition of a carbon powder coating, an appropriate increase in pressure can increase the metallization rate, improve the fluidization state, and reduce the sticking ratio. The optimal operating conditions for pure hydrogen to reduce Brazilian fine iron ore was found to be a reduction temperature of 923-1023 K, the linear velocity of the reducing gas was 0.6 m/s, the reducing time was 30-50 min, the reducing pressure was 0.25 MPa, the mass content of the coated carbon powder was 2-6% (accounting for the mass of the mineral powder), and the particle size of the carbon powder was 4-7 µm. Iron whiskers cohesion and agglomeration were the main reasons for the adhesion of ore powder particles. It was found that carbon powder coating can effectively change the morphology of metal iron, as metal iron generates spherical particles around the carbon powder to improve the fluidization state.

An Efficient Probe of Cyclometallated Phosphorescent Iridium Complex for Selective Detection of Cyanide.

A cyclometallated phosphorescent iridium-based probe to detect CN- was prepared through a cyanide alcoholize reaction based on the C^N type main ligand and N^N type ancillary ligand (2-phenyl pyridine and 1,10-phenanthroline-5-carboxaldehyde, respectively). The efficient probe exhibited good sensitivity in response to CN- in an CH3CN and H2O (95/5) mixture within a 1.23 µM detection limit. The response of PL is directly in line with the concentration of CN- from 0 to 2.0 equiv. The PL investigation of other reactive anions proved the great selectivity to CN-. Additionally, upon adding 1.0 equiv. of cyanide, the formation of cyanohydrin was correctly elucidated in 1H NMR, FT-IR, and mass spectra studies. The conspicuous results indicate that the iridium complex has the potential possibility of application in other biosystems related to CN-.