Green Energy & Environment最新文献

Removing hydrogen sulfide (H₂S) via the selective oxidation has been considered an effective way to further purify the indusial sulfur-containing due to it can completely transform residual H₂S into elemental sulfur. While N-doped porous carbon was applied to H₂S selective oxidation, a sustainable methodology for the synthesis of efficient and stable N-doped carbon catalysts remains a difficulty, limiting its future development in large-scale applications. Herein, we present porous, honeycomb-like N-doped carbon catalysts with large specific surface areas, high pyridinic N content, and numerous structural defects for H₂S selective oxidation prepared using reusable NaCl as the template. The as-prepared NC-10-800 catalyst exhibits excellent catalytic performance (sulfur formation rate of 784 g_sulfur·kg_cat.^-1·h^-1), outstanding stability (> 100 h), and excellent anti-water vapor, anti-CO₂ and anti-oxidation properties, suggesting significant potential for practical industrial application. The characterization results and kinetic study demonstrate that the large surface areas and structural defects created by the molten salt at high temperature enhance the exposure of pyridinic N sites and thus accelerate the catalytic activity. Importantly, the water-soluble NaCl template could be easily washed from the carbon nanomaterials, and thus the downstream salt-containing wastewater could be subsequently reused for the dissolution of carbon precursors. This environment-friendly, low-cost, reusable salt-template strategy has significant implications for the development of N-doped carbon catalysts for practical applications.

Emerging contaminants (ECs) are widely present in aquatic environments, posing potential risks to both ecosystems and human health. The ultrasound-assisted persulfate oxidation process has attracted considerable attention in the degradation of ECs due to its ability to generate both sulfate radicals and cavitation effects, enhancing degradation effects. In this paper, the principle of ultrasonic synergistic Fenton-like oxidation system for degrading organic pollutants was reviewed, divided into homogeneous system, non-homogeneous system, and single-atom system to explore the synergistic effect of ultrasound-enhanced persulfate technology in three aspects, and the effects of environmental factors such as ultrasonic frequency and power, system pH, temperature, and initial oxidant concentration on the system's decontamination performance were discussed. Finally, future research on ultrasonically activated persulfate technology is summarized and prospected.

Single-molecule junctions, integrating individual molecules as active components between electrodes, serve as fundamental building blocks for advanced electronic and sensing technologies. The application of ionic liquids in single-molecule junctions represents a cutting-edge and rapidly evolving field of research at the intersection of nanoscience, materials chemistry, and electronics. This review explores recent advances where ionic liquids function as electrolytes, dielectric layers, and structural elements within single-molecule junctions, reshaping charge transport, redox reactions, and molecular behaviors in these nanoscale systems. We comprehensively dissect fundamental concepts, techniques, and modulation mechanisms, elucidating the roles of ionic liquids as gates, electrochemical controllers, and interface components in single-molecule junctions. Encompassing applications from functional device construction to unraveling intricate chemical reactions, this review maps the diverse applications of ionic liquids in single-molecule junctions. Moreover, we propose critical future research topics in this field, including catalysis involving ionic liquids at the single-molecule level, functionalizing single-molecule devices using ionic liquids, and probing the structure and interactions of ionic liquids. These endeavors aim to drive technological breakthroughs in nanotechnology, energy, and quantum research.

The climate crisis necessitates the development of non-fossil energy sources. Harnessing solar energy for fuel production shows promise and offers the potential to utilize existing energy infrastructure. However, solar fuel production is in its early stages of development, constrained by low conversion efficiency and challenges in scaling up production. Concentrated solar energy (CSE) technology has matured alongside the rapid growth of solar thermal power plants. This review provides an overview of current CSE methods and solar fuel production, analyzes their integration compatibility, and delves into the theoretical mechanisms by which CSE impacts solar energy conversion efficiency and product selectivity in the context of photo-electrochemistry, thermochemistry, and photo-thermal co-catalysis for solar fuel production. The review also summarizes approaches to studying the photoelectric and photothermal effects of CSE. Lastly, it explores emerging novel CSE technology methods in the field of solar fuel production.

In recent years, porous organic catalysts have been developed and become research hotspots in photo/electrocatalysis due to their inherent pores, high specific surface area, chemical and thermal stability, and diverse functional building blocks. Phenazine-linked organic catalysts, exhibited excellent conjugation, electrical conductivity, chemical, and thermal stability, could bring in N atoms with specific numbers and positions to regulate electron levels, anchor metals, and absorb near-infrared light, which expands solar energy utilization. These advantages of the phenazine-linked catalysts attracted our group and numerous researchers to conduct experimental and computational work on photo/electrocatalytic applications and mechanisms. This review summarizes the recent significant research progress, synthesis methods, photo/electrocatalytic performance, and applications of relative phenazine-linked catalysts. Furthermore, the photo/electrocatalytic mechanism was systematized and summarized by combining experiments and density functional theory calculations simultaneously.

As a prominent contributor to air pollution, nitric oxide (NO) has emerged as a critical agent causing detrimental environmental and health ramifications. To mitigate emissions and facilitate downstream utilization, adsorption-based techniques offer a compelling approach for direct NO capture from both stationary and mobile sources. In this study, a comprehensive exploration of NO capture under oxygen-lean and oxygen-rich conditions was conducted, employing Ni ion-exchanged chabazite (CHA-type) zeolites as the adsorbents. Remarkably, Ni/Na-CHA zeolites, with Ni loadings ranging from 3 to 4 wt%, demonstrate remarkable dynamic uptake capacities and exhibit exceptional NO capture efficiencies (NO-to-Ni ratio) for both oxygen-lean (0.17–0.31 mmol/g, 0.32–0.43 of NO/Ni) and oxygen-rich (1.64–1.18 mmol/g) under ambient conditions. An NH₃ reduction methodology was designed for the regeneration of absorbents at a relatively low temperature of 673 K. Comprehensive insights into the NO_x adsorption mechanism were obtained through temperature-programmed desorption experiments, in situ Fourier transform infrared spectroscopy, and density functional theory calculations. It is unveiled that NO and NO₂ exhibit propensity to coordinate with Ni²⁺ via N-terminal or O-terminal, yielding thermally stable complexes and metastable species, respectively, while the low-temperature desorption substances are generated in close proximity to Na⁺. This study not only offers micro-level perspectives but imparts crucial insights for the advancement of capture and reduction technologies utilizing precious-metal-free materials.

Adjusting the interfacial transport efficiency of photogenerated electrons and the free energy of hydrogen adsorption through interface engineering is an effective means of improving the photocatalytic activity of semiconductor photocatalysts. Herein, hollow ZnS/NiS nanocages with ohmic contacts containing Zn vacancy (V_Zn-ZnS/NiS) are synthesized using ZIF-8 as templates. An internal electric field is constructed by Fermi level flattening to form ohmic contacts, which increase donor density and accelerate electron transport at the V_Zn-ZnS/NiS interface. The experimental and DFT results show that the tight interface and V_Zn can rearrange electrons, resulting in a higher charge density at the interface, and optimizing the Gibbs free energy of hydrogen adsorption. The optimal hydrogen production activity of V_Zn-ZnS/NiS is 10636 μmol h^-1 g^-1, which is 31.9 times that of V_Zn-ZnS. This study provides an idea for constructing sulfide heterojunctions with ohmic contacts and defects to achieve efficient photocatalytic hydrogen production.

Plasmon-induced hot-electron transfer from metal nanostructures is being intensely pursed in current photocatalytic research, however it remains elusive whether molecular-like metal clusters with excitonic behavior can be used as light-harvesting materials in solar energy utilization such as photocatalytic methanol steam reforming. In this work, we report an atomically precise Cu₁₃ cluster protected by dual ligands of thiolate and phosphine that can be viewed as the assembly of one top Cu atom and three Cu₄ tetrahedra. The Cu₁₃H₁₀(SR)₃(PR’₃)₇ (SR = 2,4-dichlorobenzenethiol, PR’₃ = P(4-FC₆H₄)₃) cluster can give rise to highly efficient light-driven activity for methanol steam reforming toward H₂ production.

Fabricating non-noble metal-based carbon air electrodes with highly efficient bifunctionality is big challenge owing to the sluggish kinetics of oxygen reduction/evolution reaction (ORR/OER). The efficient cathode catalyst is urgently needed to further improve the performance of rechargeable zinc-air batteries. Herein, an activation-doping assisted interface modification strategy is demonstrated based on freestanding integrated carbon composite (CoNiLDH@NPC) composed of wood-based N and P doped active carbon (NPC) and CoNi layer double hydroxides (CoNiLDH). In the light of its large specific surface area and unique defective structure, CoNiLDH@NPC with strong interface-coupling effect in 2D-3D micro-nanostructure exhibits outstanding bifunctionality. Such carbon composites show half-wave potential of 0.85 V for ORR, overpotential of 320 mV with current density of 10 mA cm^-2 for OER, and ultra-low gap of 0.70 V. Furthermore, highly-ordered open channels of wood provide enormous space to form abundant triple-phase boundary for accelerating the catalytic process. Consequently, Zinc-air batteries using CoNiLDH@NPC show high power density (aqueous: 263 mW cm^-2, quasi-solid-state: 65.8 mW cm^-2) and long-term stability (aqueous: 500 h, quasi-solid-state: 120 h). This integrated protocol opens a new avenue for the rational design of efficient freestanding air electrode from biomass resources.