EcoEnergy最新文献

Metal-nitrogen-doped carbon material have sparked enormous attentions as they show excellent electrocatalytic performance and provide a prototype for mechanistic understandings of electrocatalytic reactions. Researchers spare no effort to find catalytic reactivity “descriptor”, which is correlated with catalytical properties and could be utilized for guiding the rational design of high-performance catalysts. In recent years, benefited from the development of computational technology, theoretical calculation came into being as a powerful tool to understand catalytic mechanisms from an atomic level as well as to accelerate the process of finding a catalytic reactivity descriptor and promoting the development of effective catalysts. In the present review, we provide the latest theoretical research toward energetic and electronic descriptors for metal-nitrogen-doped carbon (M-N-C) materials, which have shown excellent electrocatalytic performance and provide a prototype for the mechanistic understanding of electrocatalytic reactions. This review uses density functional theory calculation and the most advanced machine learning method to describe the exploration of four kinds of electrocatalytic reaction descriptors, namely oxygen reduction reaction, carbon dioxide reduction reaction, hydrogen evolution reaction, and nitrogen reduction reaction. The aim of this review is to inspire the future design of high-efficiency M-N-C catalysts by providing in-depth insights into the electrocatalytic activity of these materials.

Nonfiltered seawater electrolysis is promising for sustainable hydrogen gas. However, hydrogen production from seawater electrolysis faces many challenges, including corrosion caused by insoluble precipitates such as Cl⁻, Mg²⁺ and Ca²⁺ in alkaline seawater as well as marine pollutants can lead to blocking active sites, together with high energy consumption, resulting in low efficiency and poor stability of electrocatalyst, which hinders the application of seawater electrolysis technology. In this work, we report H₂O enrichment of the Pt/hexagonal boron nitride (h-BN) electrocatalyst. Electrochemical tests and in situ experiments both demonstrate that h-BN as the support loaded Pt effectively prevents the corrosion of the cathode, the formation of fouling, and reduces energy consumption, resulting in prolonged operating stability at high current density. The electrocatalyst works stably for over 1000 h at a high current density of 500 mA cm⁻² in alkaline seawater electrolytes. Pt/h-BN shows better hydrogen evolution performance than Pt/C under industrial production conditions and has good industrial application prospects.

Liquid organic hydrogen carriers have emerged as promising hydrogen storage systems, offering notable advantages over conventional storage and utilization efficiency methods. However, designing a catalyst that operates at low temperatures and remains cost-effective poses a significant challenge. We successfully synthesized Pd species (single atoms, fully exposed clusters, and nanoparticles) on a nanodiamond/graphene (ND@G) hybrid support for toluene hydrogenation. The structure of as-developed Pd catalyst was investigated by HAADF-STEM, X-ray absorption fine structure, Raman, XRD, XPS, and other characterizations. Remarkably, the Pd_n/ND@G catalyst achieved a toluene conversion rate of 99.3% (100°C, 2.0 MPa H₂) without loss of catalytic ability after 5 runs, which exhibited excellent catalytic performance and stable activity. Furthermore, the Pd_n/ND@G catalyst exhibited an apparent activation energy as low as 62.36 ± 3.33 kJ mol⁻¹ and an initial turnover frequency of 33.1 h⁻¹ at 100°C. By adjusting the size and metal-dependent effects, we have achieved enhanced catalytic performance for toluene hydrogenation, thus paving the way for the design of efficient liquid organic hydrogen storage catalysts.

Ammonia (NH₃) has received significant attention due to its increasing demand as a key commodity for industrial chemical production, a green fuel, and a hydrogen (H₂) carrier. Electrochemical nitrogen (N₂) reduction reaction (ENRR) emerges as the most attractive pathway to produce NH₃. The process utilizes H₂O as a proton source under mild temperature and pressure, which can reduce CO₂ emissions and energy input compared to the traditional Haber-Bosch process. However, ENRR is severely insufficient for practical applications due to its kinetically sluggish steps compared to its competitive hydrogen evolution reaction. Also, the imbalanced reactant concentrations of N₂ and H₂O, resulting from the low N₂ solubility, and oppositely, free H₂O accessibility toward catalysts, cause the ineffective three-phase-boundary that acts as active sites for ENRR. To overcome these challenges, it is essential to perform interfacial engineering for each part of the catalyst and reaction environment. In this perspective, recent advances in interfacial engineering are examined and critically reviewed, and further research directions are proposed to develop ENRR significantly. The sections cover catalytic active site modification, hydrophobic/hydrophilic control, electrolyte engineering, and system design. The insights and prospects in this perspective will be effective for developing ENRR in a scientific and practical manner.

Dyes and antibiotics as typical persistent organic pollutants (POPs) are widely present in the environment, but can hardly be removed completely by traditional water treatment methods. Here, we designed Bi₄O₅Br₂/g-C₃N₄ composite nanosheets for efficient photocatalytic removal of POPs in water. The Bi₄O₅Br₂/g-C₃N₄ composite with a heterojunction structure exhibited high adsorption and photocatalytic activity for removal of tetracycline (TC) and ciprofloxacin (CIP) with excellent cyclic stability, owing to its large specific surface area as well as enhanced charge separation and visible light utilization. Our characterization revealed that h⁺ and ·OH are responsible for the photocatalytic degradation of TC and CIP. This work provides insights into the design of photocatalytic materials with synergy of adsorption and photocatalytic degradation, and offers a heterojunction construction strategy for addressing the increasingly severe environmental issues.

Low-dimensional mesoporous nanomaterials (LDMNs), which possess complementary properties in the mesoscale and nanoscale, have realized more technological potentials in a wide range of applications, in particular, catalysis. Although still in its infancy, the proposed monomicelles-induced assembly (MIA) has been proved to be an emerging and powerful toolbox for the direct synthesis of LDMNs with well-controlled mesostructures and architectures. This review starts from the developmental history of the MIA strategy and then discuss general protocols to fabricate the monomicelles. After that, manipulation of the monomicelles' assembly by well-designed interfaces and confined spaces for the controllable fabrication of LDMNs are reviewed in detail. Then, catalytic applications, including thermal, photo- and electrocatalysis, of LDMNs are discussed critically based on the structure-performance relationship. This review ends with a brief summary and further directions of the MIA strategy, paving the way for the synthesis of sophisticated mesoporous assemblies to achieve advanced functionalities.

Increasing global environmental deterioration is becoming a serious concern, leading to an exponential increase in scientific interest in renewable energy as an alternative to replace fossil fuels. Photoelectrochemical (PEC) water splitting, which directly converts sunlight into hydrogen fuel, offers a promising renewable energy technology. Semiconductors, used as photoelectrodes, provide the most feasible method for converting solar energy into electrical energy and chemical fuels. Unfortunately, most of the common semiconductors used in PEC water splitting have wide bandgaps, which greatly restrict the utilization efficiency of sunlight. To promote the solar-to-hydrogen (STH) efficiency of PEC water splitting, atomically precise clusters with regular crystal structures have been introduced in the PEC systems. In this review, the recent advances in nanoclusters for PEC water splitting, including metal clusters, polyoxometalates, semiconductor clusters, and carbon clusters, are summarized. At last, major challenges and outlook for the development of clusters for PEC water splitting are provided.

Graphdiyne (GDY), a new carbon allotrope containing sp and sp²-hybridized carbon atoms, features the one-atom-thick two-dimensional structure with many unique and promising characteristics, such as highly conjugated and extremely large π structures, abundant carbon chemical bonds, naturally distributed pores, inherent band gap, excellent chemical and mechanical stability, highly uneven distributed surface charges, and can be grown on the surface of arbitrary substrates. GDY has been one of the hottest frontiers in chemistry and material sciences and represents a new development trend and research direction in the development of carbon materials. Owing to the unique characteristics in chemical and electronic structures, GDY has shown great application potentials and prospects in many fields, including catalysis, energy, optoelectronics, life science, and intelligent device. In this review, the structures, synthetic methods, and fundamental properties of GDY are introduced. In particular, the recent advances of GDY and its formed aggregates in hydrogen energy conversion are summarized and discussed.

Hydrogen produced from electrocatalytic water splitting means is deemed to be a promising route to construct a low-carbon, eco-friendly, and high-efficiency modern energy system. The design and construction of highly active catalysts with affordable prices toward alkaline hydrogen evolution reaction (HER) are effective in accelerating the overall water-splitting process. So far, ruthenium (Ru) based catalysts deliver comparable or even superior catalytic performance relative to the platinum (Pt)/C benchmark. Combined with their price advantage, Ru-based catalysts are undoubtedly considered as one of the perfect alternatives of Pt toward the alkaline HER. Extensive efforts have been made to reasonably synthesize Ru-related materials, but a careful insight into material engineering strategies and induced effects remain in its infancy. In this review, recent progress on the material engineering strategies for improving the catalytic activity of Ru-related catalysts, including electronic regulation, geometric modulation, local structure alteration, self-optimization strategies, and the induced structure–activity relationship are comprehensively summarized. Furthermore, the challenges and perspectives on future studies of Ru-related electrocatalysts for the alkaline HER are also proposed.

Electrocatalytic N₂ reduction (NRR) has been regarded as a promising approach for environment-friendly and sustainable ammonia (NH₃) synthesis. However, developing cost-effective electrocatalysts with high NRR efficiency at low overpotential in neutral media remains a great challenge. In this paper, a freestanding NRR electrocatalyst, BiFeO/FCC, has been developed by in situ growth of bismuth ferrite (Bi₂₅FeO₄₀) on functionalized carbon cloth (FCC), which exhibits high NRR activity with a maximum NH₃ yield of 3.88 μg h⁻¹ cm⁻² (at −0.40 V vs. reversible hydrogen electrode [RHE]) and a Faradaic efficiency of 12.71% (at −0.45 V vs. RHE) in 0.1 M Na₂SO₄. The synergistic effect of the abundant exposed bismuth and iron dual active sites confined in the lattice, the binder-free nature of the electrode and the excellent conductivity of the carbon substrate enable the easy adsorption/activation of N₂ and accelerate the electron transfer simultaneously, thus boosting its NRR performance. This work is significant to design low-cost, and high-efficient NRR catalysts for large-scale electrocatalytic NH₃ synthesis.