Broad Absorption Research Articles

When cellulose nanocrystals meet graphene oxide: Structurally enhanced aerogels for efficient solar steam generation and water purification

Pollution, population growth, and climate change are intensifying global freshwater shortages. Traditional methods of collecting freshwater, such as rainwater harvesting and sewage treatment, have high energy consumption, limiting their implementation in underdeveloped regions. On the other hand, solar-driven seawater evaporation offers a promising solution, purifying water using naturally abundant solar energy. Reduced graphene oxide (rGO) is considered as a strong candidate for this purpose due to its broad spectral absorption. However, its hydrophobicity hinders its direct use in solar steam generators. Here, we report the preparation of a series of cellulose nanocrystal (CNC)-rGO aerogels (CGAs) through a one-pot hydrothermal gelation process, followed by unidirectional freeze-drying. The introduction of CNCs enhances the hydrophilicity and structural stability of the resulting CGAs. The CGAs also feature uniform and unidirectional channels that promote efficient water transport, as confirmed by scanning electron microscopy (SEM) and X-ray microtomography (XMT). The CGAs have an optimized water evaporation rate of 1.80 kg m−2 h−1 under 1 sun irradiation, with 90 % solar-to-vapor energy efficiency. Moreover, durability and seawater desalination tests provide additional evidence for the practicality of CGAs in water purification. It is anticipated the implementation of CGAs will expedite the application of solar steam generators in practical scenarios.

Broad microwave absorption bandwidth analysis of biocomposite microwave absorber material for X-band applications

Broad microwave absorption bandwidth analysis of biocomposite microwave absorber material for X-band applications

First-principles study of GeC/Ga2SO heterostructure as a potential direct Z-scheme photocatalyst for water splitting

The rational design of van der Waals heterostructure offers an effective avenue for improving the photocatalytic efficiency of individual two-dimensional materials, garnering extensive interest in recent years. Herein, the feasibility of GeC/Ga2SO heterostructure as a photocatalyst for overall water splitting has been explored based on the first-principles calculations. Our findings reveal that the electronic bandstructure of GeC/Ga2SO heterostructure can be engineered in staggered or straddling band alignment depending on stacking patterns. Particularly, in the GeC/Ga2SO heterostructure with staggered band alignment, an intrinsic built-in electric field is established at the interface with the direction from GeC to Ga2SO, facilitating the formation of a direct Z-scheme heterostructure. Also importantly, the band-edge positions of Z-scheme GeC/Ga2SO heterostructure cross the water redox potentials, providing adequate driving force for both the reduction and oxidation reactions of water. Gibbs free energy calculations demonstrated that the photocatalytic overall water splitting can proceed spontaneously in the neutral environment (pH = 7) under light irradiation. Moreover, GeC/Ga2SO heterostructure exhibits good thermal stability and a strong (magnitude in 105 cm−1) and broad (from visible to ultraviolet light) optical absorption. Finally, through applying the tensile strain, further enhancements in the optical absorption and carrier redox ability are achieved due to the favorable modulation in the bandgap. Therefore, all these features make GeC/Ga2SO heterostructure show great potential in the application of photocatalytic water splitting.

2D sp2 carbon-linked benzotrithiophene covalent organic frameworks for selective sulfoxidation with oxygen driven by green light

Covalent organic frameworks (COFs) are promising photocatalysts with excellent chemical stability, broad light absorption, and tailorable molecular structures. To assemble highly crystalline 2D (two-dimensional) COFs, planar molecular units like benzotrithiophene (BTT) and 2,2′-bipyridine (Bpy) are highly desired. Herein, two COFs are assembled by the condensation of benzo[1,2-b:3,4-b′:5,6-b′′]trithiophene-2,5,8-tricarbaldehyde with [2,2′-bipyridine]-5,5′-diacetonitrile and [2,2′-bipyridine]-5,5′-diamine, respectively. An sp2 carbon-linked COF Bpy-sp2c-BTT-COF and an imine-linked COF Bpy-IM-BTT-COF with apparent electron donor–acceptor configuration are readily furnished in which the planarity of Bpy underpins their crystallinity. The sp2-carbon linkage is more essential than the imine linkage in adjusting band structure and facilitating electron transfer over Bpy-sp2c-BTT-COF and Bpy-IM-BTT-COF. Therefore, Bpy-sp2c-BTT-COF demonstrates better performance than Bpy-IM-BTT-COF for selective sulfoxidation with oxygen driven by green light in which superoxide and single oxygen are both involved during the activation of oxygen. The linkage selection for COFs opens new doors into visible light photocatalysts for selective conversions.

A π−π stacked porous framework for highly efficient second near-infrared photothermal effects and photo-thermo-electric conversion

Near-infrared (NIR) photothermal compounds, which convert low-energy NIR photons into heat, have recently attracted significant attention due to their potential applications in many areas such as photothermal imaging, diagnosis and therapy, photosensors, and catalysis. Photothermal conversion efficiency (PCE), a critical parameter of NIR photothermal materials, significantly influences their practical performance. However, exploring highly efficient NIR photothermal compounds, particularly in the NIR-II domain, remains a significant challenge. Herein, we report on a highly efficient NIR-II photothermal compound based on a novel π−π stacked porous framework {[Ni4Cl2(ONDI)2(bpy)4]⋅2Cl⋅2H2O⋅xDMF⋅yH2O}n (1). This compound features a porous supramolecular framework constructed through intermolecular π−π interactions. Additionally, compound 1 exhibits broad optical absorption spanning from the ultraviolet to the NIR region, with an edge extending to 1600 nm. Under irradiation with a 1064 nm laser, compound 1 demonstrates significant NIR-II photothermal effects, achieving a remarkable PCE of 84.4 %, attributed to the formation of charge states and the abundant π−π interactions in its crystal structure. When integrated with commercial thermoelectric generators, compound 1 shows promising potential for photo-thermo-electric conversion, with a maximum open-circuit voltage of 250 mV and 350 mV under irradiation of 1 sun and 2 suns, respectively. Furthermore, the output power density of 1@TEC1-12701 reaches 0.53 W/m2 under 1 sun and 1.23 W/m2 under 2 suns.

A novel triple-signal biosensor based on ZrFe-MOF@PtNPs for ultrasensitive aflatoxins detection

The development of more sensitive, stable, and portable biosensors is crucial for meeting the growing demands of diverse and complex detection environments. MOF-based nanozymes have emerged as excellent optical reporters, making them ideal signal donors for constructing multi-signal lateral flow immunoassays (LFIA). In this study, a ZrFe-MOF@PtNPs nanocomposite was synthesized by uniformly depositing platinum nanoparticles (PtNPs) onto the surface of ZrFe-MOFs using an impregnation-reduction method. The ZrFe-MOF@PtNPs exhibited broad absorption spectra, excellent peroxidase-like activity (SA = 21.77 U/mg), high solvent stability, and efficient antibody binding capability. A portable LFIA platform was developed based on ZrFe-MOF@PtNPs and a smartphone for the targeted detection of carcinogenic aflatoxins. This method enabled the readout of colorimetric, fluorescent, and catalytic signals, significantly enhancing detection sensitivity, ensuring result accuracy, and expanding the dynamic detection range. For aflatoxin M1, the calculation of the detection limit of the three signal modes reached as low as 0.0062 ng/mL, which is two orders of magnitude more sensitive than AuNPs-LFIA (0.1839 ng/mL). This study provides effective guidance for multifunctional modification of MOFs and serves as a reference for the application of MOF-based nanozymes in point-of-care biosensors.

Theoretical Insight into Fluorination on Low‐Cost A‐π‐D‐π‐A Type Donor Materials for All‐Small‐Molecule Organic Photovoltaic Cells

Low‐cost organic photovoltaic (OPV) devices have shown enormous potential in large‐scale industrial applications. And it has attracted widespread attention in the past few decades. However, the photophysical characteristics of these budget‐friendly materials haven't been explored much. Here, low‐cost small materials, including small molecule 1 (asm1) with ortho‐fluorinated side chain and small molecule 2 (asm2) with meta‐fluorinated side chain were selected to probe the fluorination effect on the absorption spectra, electrochemical energy levels, electrostatic potential (ESP), etc. The results show that the molecules asm1 and asm2 have good planarity of the backbone. And the meta‐fluorinated side chain of asm2 contributes more to the highest occupied molecular orbital and less to the lowest unoccupied molecular orbital than asm1. Moreover, differences in ESP are found between donor and acceptor materials. Furthermore, strong and broad light absorption in the visible region of these low‐cost molecules is observed, resulting in a better short‐circuit current density for the devices constructed by the donors asm1, asm2, and acceptor Y6. In addition, more charge transfer mechanisms are characterized for the asm1/Y6 system. The introduction of ortho‐fluorination in the conjugated side chain of the molecule is a favorable approach, which will provide theoretical guidance for further molecular design experiments.

Enhanced charge carrier separation and stable photoelectrochemical water splitting via a high-performance BiVO4/BiOBr Type-II heterojunction

The development of an ideal photoanode that exhibits broad light absorption, efficient photogenerated carrier separation, and superior transmission efficiency remains a pivotal challenge in enhancing the sluggish photoelectrochemical (PEC) water splitting reaction. Here, we present an efficacious strategy to bolster the PEC performance of oxygen evolution by fabricating a BiVO4/BiOBr heterojunction through a combined electrochemical deposition-calcination approach and the successive ionic layer adsorption and reaction (SILAR) method. The band structure of BiOBr is optimally aligned with BiVO4, enabling the heterojunction to significantly enhance the separation efficiency of photogenerated charges and accelerate the kinetics of PEC water oxidation. Under simulated sunlight irradiation, the BiVO4/BiOBr heterojunction exhibits a remarkable photocurrent density of 2.69 mA/cm2 at 1.23 V vs. reversible hydrogen electrode (RHE), surpassing the performance of bare BiVO4 film (0.46 mA/cm2 at 1.23 V vs. RHE) and demonstrating exceptional stability. This work offers novel insights into the rational design and fabrication of solar-driven PEC water splitting photoanodes.

Enhancing broadband absorption and photocurrent generation in carbon dots via P3HT integration

The growing interest in carbon dots (CDs) arises from their diverse applications and unique properties. This study addresses challenges in CDs for photodetector (PD) applications, specifically surface defects and trap states hindering efficient charge transport. CDs/P3HT composites were prepared to overcome these issues by incorporating CDs in a poly(3-hexylthiophene) (P3HT) matrix. Broad absorption in spectroscopic characterization revealed its utility in fabricating a broadband PD. The CDs/P3HT PD displays a remarkable broadband photoresponse, spanning both UV and visible regions. The CDs and P3HT are effectively combined via non-covalent π-π interactions constituted by their conjugated systems. The π-π interaction increases electron delocalization and facilitates efficient charge transfer due to band alignment at the junction interface. Hence, fabricated CDs/P3HT PD demonstrated enhanced photocurrent compared to pure CDs, exhibiting high responsivity of 6.12 × 10−3 AW−1 and detectivity of 0.69 × 109 Jones. This study highlights the potential of CD/P3HT composites for broadband photodetector applications with enhanced photoelectric conversion.

Highly efficiency up and down -conversion photoluminescence in Er/Tm/Yb co-doped lutecia-stabilized zirconia single crystals

High-quality transparent cubic lutecia-stabilized zirconia and LSZ:Yb1Er0.05Tm0.5 single crystals were grown by the optical floating zone method for the first time. For comparison, YSZ and YSZ:Yb1Er0.05Tm0.5 single crystals were also grown. No absorption peaks were observed in the 200 ∼1100 nm range in the transmission and absorption spectra of LSZ and YSZ, indicating that both crystals are excellent matrix crystals. The absorption spectra of LSZ:Yb1Er0.05Tm0.5 and YSZ:Yb1Er0.05Tm0.5 crystals exhibit several absorption peaks at 377, 408, 462, 488, 516, 679, 785 nm and a strong broad absorption band in the 836 ∼ 1050 nm range. The up-conversion photoluminescence of the LSZ:Yb1Er0.05Tm0.5 crystal excited by a 980 nm laser exhibited several distinct emission peaks at 300, 372, 476, 531, 548, 642 and 798 nm; similar emission peaks were observed in the up-conversion photoluminescence spectrum of the YSZ:Yb1Er0.05Tm0.5 crystal, except for the absence of the 300 nm peak. The intensity of the emission peaks of the former was higher than that of the corresponding peaks of the latter. Power curves indicated that the 300 nm emission is a four-photon up-conversion process, the 372 nm and 476 nm emissions are three-photon processes, and the 548 nm and 642 nm emissions are two-photon processes. Under excitation at 379 nm, the down-conversion photoluminescence spectra of the LSZ:Yb1Er0.05Tm0.5 and YSZ:Yb1Er0.05Tm0.5 crystals showed emission peaks at 450, 457, 511, 531 and 637 nm, the peak intensities of the former are higher than those of the latter, which is due to the former with higher density and lower phonon energy as compare to the latter. These results indicate that LSZ:Yb1Er0.05Tm0.5 single crystal has advantages over YSZ:Yb1Er0.05Tm0.5 single crystal for luminescence in photonic devices.

Investigation into the carrier recombination in Sb2Se3: Photo thermal effect, trapped carrier absorption and hot carrier cooling

Understanding the carrier recombination processes in Sb2Se3 is essential for its optoelectronic applications. In this work, carrier recombination dynamics in Sb2Se3 were studied by broad band transient absorption spectroscopy. Firstly, the contribution of photothermal effect to the transient absorption spectrum was thoroughly discussed. It is confirmed that the excited state absorption (ESA) band with lifetime of several nanoseconds results from co-contribution of photo thermal effect and deep trapped carrier absorption. Secondly, the features of transient absorption spectrum on picosecond time scale were interpreted. The short-lived ESA band around 1000 nm was assigned to shallow trapped carrier absorption, while not band gap renormalization (BGR) or free carrier absorption. By globally fitting the transient absorption spectrum, the hot carrier cooling time and time constant for free carrier relax into deep trap state were determined to be 0.25∼0.45 ps and 3.1∼8.7 ps, respectively. Finally, we built up the carrier recombination model of Sb2Se3. The experimental results in this work will improve the understanding on the carrier recombination in Sb2Se3.

Advancing environmental remediation through tailored TiO2 nanomaterials in water and air purification

This study investigates the green synthesis of TiO2 nanoparticles at varying concentrations (0 %, 0.1 %, 2.5 %, 5 %, and 10 %) using Viola betonicifolia plant extract, focusing on their application in environmental purification, specifically in water and air decontamination. X-ray diffraction (XRD) analysis confirmed the anatase crystal structure of TiO2 nanoparticles, with an average crystallite size of approximately 22 nm. Transmission electron microscopy (TEM) revealed a median diameter of around 22 nm, corroborating the findings from XRD. The effectiveness of these TiO2 nanomaterials was evaluated through bench-scale models simulating real-world conditions, targeting a broad range of pollutants, including heavy metals, organic dyes, volatile organic compounds (VOCs), and microbial pathogens. Advanced analytical techniques such as High-performance liquid chromatography (HPLC), Inductively coupled plasma mass spectrometry (ICP-MS), and microbial plate count methods quantified the pollutant removal efficiency, demonstrating the significant potential of the synthesized TiO2 nanoparticles. Dynamic light scattering (DLS) analysis showed a mean hydrodynamic diameter of 22 nm and a polydispersity index (PDI) below 0.1, indicating a uniform size distribution. The FTIR spectrum revealed a broad absorption band at 3400 cm−1, corresponding to O–H stretching vibrations, indicative of hydroxyl groups crucial for the photocatalytic activity of TiO2. The UV–visible spectroscopy indicated a maximum absorption at 642 nm, associated with the п-п* transition. Photocatalytic degradation of methylene blue under UV irradiation achieved a degradation efficiency of 94 % after 120 min, underscoring the superior efficiency of the green synthesis method.

Designing a hollow MoSe2/CuS nanospheres type-II heterojunction photocatalyst with superior UV-vis-NIR absorption for photocatalytic degradation of organic pollutants.

In this work, a hollow MoSe2/CuS type-II heterojunction was fabricated using hollow MoSe2 nanospheres as the basis for structural design. UV-Vis-NIR diffuse absorption tests show that MoSe2/CuS has a broad spectral absorption to extend the optical response range from UV-Vis to NIR. The light source utilization rate and interfacial area are increased by the hollow MoSe2/CuS core-shell structure. The broad absorption ability of MoSe2/CuS can facilitate the photocatalysis process. As the electrochemical impedance of MoSe2/CuS is lower than that of the MoSe2, MoSe2/CuS has a good photogenerated carrier separation efficiency. Benefiting from the synergistic facilitation effect of the multi-level 3D hollow nanosphere and the significant space charge region in type-II heterojunction, the RhB degradation efficiency of MoSe2/CuS reached 96.0% in 120.0minunder Xe (350W) broadband spectrum light irradiation. The photocatalysis mechanism of the hollow MoSe2/CuS core-shell structure was investigated. This work provides an insight into the application of broad spectrum semiconductor heterojunctions to solve environmental problems.

Modulating intramolecular charge transfer via π-d conjugative effect in coordination polymers toward photo-thermo-electric conversion

The prospect of harnessing sunlight to generate cost-effective heat and electricity presents a captivating opportunity to address water scarcity and electricity shortages. Photothermal materials with a broad absorption spectrum are indispensable for effectively harnessing solar energy and converting it into heat/electricity. Herein, we developed an intramolecular charge transfer strategy via conjugated effect to regulate solar absorption and photothermal conversion ability of M-DABDT (M = Fe/Co/Ni/Cu/Zn, DABDT = 2,5-diaminobenzene-1,4-dithiol), overcoming a common limitation of narrow absorption and low photothermal efficiency in traditional metal-organic assemblies. The density functional theory calculations reveal that altering transition metal ions induces the structural torsion of organic linkers, resulting in a significant change in dihedral angle from 89.96° to 2.57°. The structural change significantly facilitates the charge transfer and electron relaxation, ultimately promoting the conversion of light to heat. Under one sun irradiation, the maximum temperature of Fe-DABDT can reach approximately 92.5 ℃. More significantly, the integration of M-DABDT CPs and thermoelectric devices under normal solar irradiation results in an extraordinary open circuit voltage (238 mV) and maximum power density (364.5 μW m−2), processing a peak output voltage density of 76.9 V m−2 at 11:00 a.m. in the presence of outdoor sunlight. This strategy presents an avenue for developing metal-organic solar absorbers for photo-thermo-electric conversion systems.

Hierarchical porous molybdenum carbide synergic morphological engineering towards broad multi-band tunable microwave absorption

Hierarchical porous molybdenum carbide synergic morphological engineering towards broad multi-band tunable microwave absorption

Benzodiazole-Based Covalent Organic Frameworks for Enhanced Photocatalytic Dehalogenation of Phenacyl Bromide Derivatives.

Covalent organic frameworks (COFs) have garnered significant interest within the scientific community due to their distinctive ability to act as organic semiconductors responsive to visible light. This unique attribute makes them up-and-coming candidates for facilitating photocatalytic organic reactions. Herein, two donor-acceptor COFs, TPE-BSD-COF and TPE-BD-COF, have been designed and synthesized by incorporating electron-rich tetraphenylethylene and electron-deficient benzoselenadiazole and benzothiadiazole units into the framework through a Schiff-base polycondensation reaction. Both COFs exhibit exceptional crystallinity and enduring porosity. TPE-BSD-COF and TPE-BD-COF exhibit broad light absorption capabilities, a narrow optical band gap, and low electrochemical impedance spectrum (EIS) levels, indicating that the two COFs are effective heterogeneous photocatalysts for the reductive dehalogenation of phenacyl bromide derivatives under blue LED irradiation. A high photocatalytic yield of 98% and 95% was achieved by TPE-BSD-COF and TPE-BD-COF catalysts, respectively, within only one hour.

Achieving efficient electromagnetic absorption in multifunctional carbon nanotube aerogels by manipulating radialized network structure

The rapid advancements in communication technology have greatly propelled the widespread applications of artificial intelligence (AI). While AI technology facilitates society, it also brings the unavoidable electromagnetic hazards and the issue of disposal of electronic plastic wastes. So, utilizing electronic plastic wastes to constructing carbon-based electromagnetic wave (EMW) absorption materials, are highly promising. However, how to use CNTs from plastic wastes to build good EMW absorption performance aerogels is a critical challenge. In this work, highly porous and well-interconnected network aerogels constructed by radialized CNT arrays are rationally designed under the guidance of grave-to-cradle strategy, exhibiting altered impedance matching and multiple EMW attenuation methods. Theoretical calculations suggest that a well-designed heterojunction interface structure can enhance the conductivity and interface polarization of CNTAs. The CNT aerogels (CNTAs) realize broad absorption bandwidth covering 8.48 GHz with a minimum reflection loss of −59.5 dB. Moreover, the radialized arrays network of CNTAs also endows it with electromagnetic protection, thermal management, self-cleaning, and air purification functions. These inspiring achievements of multifunctional CNTA-2 provides new help for the safe and stable promotion of the AI era.

Computational insight on K2AuBiX6 (X = F, Cl, Br, I) double perovskites to comprehensively investigate mechanical, optoelectronic, and thermoelectric features for green energy applications

In this article, we investigated the structural, elastic, electronic, optical, and thermoelectriccharacteristics of K2AuBiX6 (X = F, Cl, Br, and I) using density functional theory (DFT). To verify the stability of the cubic structure tolerance, octahedral factors, and formation energy have been determined. The mechanical stability has been governed by Born stability criteria. These parameters ensure its strength, ductility, brittleness, and anisotropy. The bandgaps of K2AuBiF6, K2AuBiCl6, K2AuBiBr6, and K2AuBiI6 have been determined using the TB-mBJ potential. The calculated values of energy band gaps are 2.88, 2.02, 1.38, and 0.95 eV, respectively. These materials exhibit a broad absorption in visible regions, a refractive index range of around 1–3, and low light scattering, which makes them ideal for optoelectronic applications. In addition, the figure of merit (ZT) values for these compounds at room temperature are 0.76, 0.78, 0.77, and 0.80, ensuring their suitability for use in thermal devices.

Graphene with suitable-size nitrogen-doped cavity being an excellent photocatalyst for proton-coupled electron transfer in water splitting

Aiming to attain porous carbon nitride photocatalysts with high specific surface area, abundant active sites, broad absorption range and effective electron-hole separation, we remove carbon rings from graphene and replace all the edge carbon atoms of the cavity with nitrogen atoms. The accurate electronic structures and exciton properties of the proposed materials are revealed by the ab initio many-body Green's function theory. Computational results show that the absorption of the designed materials can cover both the visible and the near-infrared light region. The exciton binding energies of the materials are one order of magnitude lower than those of the typical two-dimensional photocatalyst graphitic carbon nitride. Due to the formation of hydrogen bonds between pyridinic nitrogen atoms and water molecules during water splitting, the key excited-state proton-coupled electron transfer reactions are barrierless. These findings could serve as guidelines for the realization of high-performance metal-free two-dimensional photocatalysts.

Synthesis and characterization of novel yellow-green Cr, Zn-codoped Ba(Mg6Ti6)O19 pigments with high NIR reflectance

This work reports a series of yellow-green near-infrared (NIR) reflective pigments, Ba(Mg6-x-yZnyTi6-xCr2x)O19 (x = 0–1.0, y = 0–2.5), with strong NIR reflectivity for solar thermal energy regulation. Comprehensive analyses were carried out to characterize the obtained pigments including X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy, UV–Vis–NIR spectrophotometry, and CIE L*a*b* color measurement. Absorption spectra of Ba(Mg6-xTi6-xCr2x)O19 showed that the yellow-green absorption is attributed to the octahedrally coordinated Cr3+ with d-d electron transitions of 4A2(F)→4T1(F) and 4A2(F)→4T2(F). However, their broad absorption peak centered at 1200 nm severely deteriorated the insulating properties of the pigments. Through substituting Mg with Zn, the obtained pigment Ba(Mg2.5Zn2.5Ti5Cr2)O19 showed an excellent NIR solar reflectance (R* = 67 %) with color performances (L* = 61.98, a* = −18.72, b* = 22.23). EnergyPlus simulation results show that for a warm city (Haikou), the Ba(Mg2.5Zn2.5Ti5Cr2)O19 coating for the external surface of a model house (TSR = 35 %, R* = 55 %) can reduce annual cooling energy consumption by 8 % of the house.