Search

Cu3SbSe4, a copper-based sulfide free of rare earth elements, has received extensive attention in thermoelectric materials. However, its low carrier concentration restricts its widespread application. In this study, a microwave-assisted solution synthesis method was used to produce samples of Cu3SbSe4, which enabled the formation of CuSe in situ and increased the yield. Through the use of first-principles calculations, structural analysis, and performance evaluation, it was found that CuSe can enhance the carrier concentration and that induced nano-defects have a positive effect on reducing the lattice thermal conductivity. Moreover, doping with Sn decreases the band gap of the system and moves the Fermi level into the valence band, increasing the carrier concentration to 1.15 × 10−20 cm−3. Finally, the zT value of the Cu3Sb0.98Sn0.02Se4 sample was achieved at 1.05 at 623 K when the theoretical yield of a single synthesis was 10 mmol.

In aqueous electrolytes, the uncontrollable interfacial evolution caused by a series of factors such as pH variation and unregulated Zn2+ diffusion would usually result in the rapid failure of metallic Zn anode. Considering the high correlation among various triggers that induce the anode deterioration, a synergistic modulation strategy based on electrolyte modification is developed. Benefitting from the unique pH buffer mechanism of the electrolyte additive and its capability to in situ construct a zincophilic solid interface, this synergistic effect can comprehensively manage the thermodynamic and kinetic properties of Zn anode by inhibiting the pH variation and parasitic side reactions, accelerating de‐solvation of hydrated Zn2+, and regulating the diffusion behavior of Zn2+ to realize uniform Zn deposition. Thus, the modified Zn anode can achieve an impressive lifespan at ultra‐high current density and areal capacity, operating stably for 609 and 209 hours at 20 mA cm−2, 20 mAh cm−2 and 40 mA cm−2, 20 mAh cm−2, respectively. Based on this exceptional performance, high loading Zn||NH4V4O10 batteries can achieve excellent cycle stability and rate performance. Compared with those previously reported single pH buffer strategies, the synergistic modulation concept is expected to provide a new approach for highly stable Zn anode in aqueous zinc‐ion batteries. [ABSTRACT FROM AUTHOR]

Synergistic modulation has been extensively explored to develop highly efficient transition-metal-based electrocatalysts for oxygen evolution reaction (OER) because coupling effects among intrinsic activity, conductivity, mass transfer, mass diffusion, and intermediates adsorption can further promote catalytic activity. In this review, recent progress in both experimental and theoretical research on synergistic modulation for transition-metal-based alkaline OER electrocatalysts is focused. Specifically, synergistic effects will be presented in the following aspects: (1) metal reactive sites and heterogeneous atoms; (2) heterogeneous atoms and crystallographic structure; (3) electronic structure and morphology; (4) elementary reaction steps; and (5) external fields. Finally, the remaining challenges and prospects of synergistic modulation for efficient OER are further proposed. [ABSTRACT FROM AUTHOR]

The previous works commonly adjust the carrier concentration through acceptor doping, but at the same time, the decrease of the Seebeck coefficient limits the further improvement of electrical properties in Cu3SbSe4-based materials. In this work, a microwave-assisted hydrothermal synthesis method was used to synthesize Cu3SbSe4/TiO2 hollow microspheres. Part of TiO2 participates in the reaction, replaces the Sb site of Cu3SbSe4 to form holes, and the rest is dispersed in the matrix in the form of the second phase. The first-principles calculations reveal that the doping of Ti significantly changes the band structure and phonon spectrum, thereby regulating carrier concentration while increasing phonon scattering. In addition, experimental results show that the energy filtering effect generated by the extra-mixed TiO2 nano particles, which suppresses the decrease of Seebeck coefficient by acceptor doping. Consequently, the highest average power factor 897.5 μW m−1 K−2 and the zT peak value of 0.70 can be obtained in Cu3SbSe4/6%TiO2 sample at 298–623 K. This work provides a new sight to improve the thermoelectric properties in Cu3SbSe4 through carrier concentration regulation and nano-phase composition.

The medical applications of camellia oil are limited due to the instability of its active ingredients throughout the digestive tract. Pickering emulsion is one of the promising strategies to address this issue, yet the synergistic effect of oil and emulsifier phases on modulation of human gut microbiota is still unclear. Herein, high crystallinity rod-like bamboo nanocellulose (BNC) with a major diameter of 100–170 nm was prepared. BNC served as emulsifier to stabilize camellia oil emulsion and allowed for a stable storage period of more than 70 days at 4 °C. The BNC loading and ratio of water/oil attributed important effects on emulsion stability. During the investigations interrogating fermentation by gut microbiota in vitro , the concentrations of SCFAs (n -valeric, i -butyric, and i -valeric acids) were elevated in the emulsion treated groups. Additionally, proliferation of Dorea and Phascolarctobacterium , and inhibition of Desulfovibrio and Bacteroides were the key features through the emulsion intervention. Functional metabolic pathway analysis demonstrated the significant enhancement in carbohydrate metabolism and membrane transport. These findings suggested that insoluble BNC-stabilized camellia oil emulsion could be used as a dietary collocation for potential applications involving medical delivery system and synergistic modulation of gut microbiota. • Bamboo nanocellulose stabilized camellia oil emulsion was prepared with a 70-day stable storage period. • Mechanism on synergistic regulation of gut microbiota by bamboo cellulose and camellia oil was elucidated. • Bamboo cellulose properties and metric changes during storage were taken into explanation of emulsion stability. [ABSTRACT FROM AUTHOR]

• A novel patterned composite film is designed for thermal control smart windows. • This patterned Fabry-Pérot resonant structure can achieve dual-band coordinated regulation of sunlight and thermal radiation. • The optimized composite film has excellent optical properties, with T lum-L =50.4 %, Δ T sol = 13.9 % and Δ ε LWIR =0.49. • The physical mechanismthe is elucidated through the analysis of the electric field. Vanadium dioxide (VO 2) emerges as promising material for smart windows due to its ability to dynamically modulate the characteristics of near-infrared light during phase transition, accompanied by a relatively high luminous transmittance (T lum). However, traditional VO 2 -based smart windows have predominantly emphasized achieving high solar modulation ability (Δ T sol), often overlooking the modulation of emissivity (ε) of long-wave infrared (LWIR). This oversight makes it challenging to achieve optimal energy-saving effects. To address this, patterned smart window composite films are designed and optimized by using Fabry-Pérot cavity to achieve dual-band coordinated regulation of sunlight and thermal radiation, which can greatly improve the energy-saving efficiency. The obtained composite film has a great low-temperature luminous transmittance (T lum-L =50.4 %) and a high solar modulation ability (Δ T sol = 13.9 %). Meanwhile, the composite film can adaptively adjust its emissivity, with emissivity values of 0.67 and 0.18 at high and low temperatures, respectively, endowing it with excellent thermal radiation regulation capabilities. The development of patterned composite films is of great significance in the field of thermal control smart windows, which has great potential in improving the energy efficiency of buildings and enhancing resident comfort. [ABSTRACT FROM AUTHOR]

Tin perovskites present promising alternatives to lead perovskites, offering comparable optoelectronic properties alongside environmentally friendly characteristics. However, the rapid crystallization and easy oxidation of Sn 2+ lead to poor film quality, further constraining the device performance. Here, 4-hydroxypyridine (4-HP) is introduced into the tin perovskite precursor for fabrication of high-quality tin perovskite films. 4-HP could modulate the colloidal size of prenucleation perovskite clusters in the precursor, thus inducing fast nucleation and retarding the crystal growth rate of tin perovskite through the formation of chemical interaction between nitrogen of pyridine and Sn 2+ ions. Furthermore, the hydroxyl group on the pyridine ring contributes to suppressing the oxidation of Sn 2+ . As a result, the power conversion efficiency (PCE) of the devices based on 4-HP increases up to 11.3%. The stability of the unencapsulated devices shows significant improvement, retaining 100% of their initial PCEs after 2000 h of storage in N 2 with 50-100 ppm of O 2 . This research presents a novel approach to the synchronized regulation of tin perovskite crystallization and the suppression of Sn 2+ oxidation.

Synergistic modulation has been extensively explored to develop highly efficient transition-metal-based electrocatalysts for oxygen evolution reaction (OER) because coupling effects among intrinsic activity, conductivity, mass transfer, mass diffusion, and intermediates adsorption can further promote catalytic activity. In this review, recent progress in both experimental and theoretical research on synergistic modulation for transition-metal-based alkaline OER electrocatalysts is focused. Specifically, synergistic effects will be presented in the following aspects: (1) metal reactive sites and heterogeneous atoms; (2) heterogeneous atoms and crystallographic structure; (3) electronic structure and morphology; (4) elementary reaction steps; and (5) external fields. Finally, the remaining challenges and prospects of synergistic modulation for efficient OER are further proposed.

Neuromorphic devices are of great significance for next generation energy-efficient brain-like computing and perception. Oxide-based photoelectric neuromorphic transistors are very promising due to the proton-related electric-double-layer (EDL) effect and persistent photoconductivity behavior. In this study, indium-gallium-zinc-oxide (IGZO)-based photoelectric neuromorphic thin-film transistors (TFTs) with tunable synaptic plasticity are proposed. Some important synaptic functions, such as excitatory postsynaptic current, multipulse facilitation, and long-term plasticity, can be effectively tuned by the photoelectric synergistic modulation. More importantly, under the photoelectric synergistic modulation, the temporary short-term memory can be converted into permanent long-term memory. And the voltage coordinated modulation can enhance the image in the pixel and the ability of real-time data processing of the input visual information. Our results are very important for the development of photoelectric neuromorphic devices with configurable dynamic functions. [ABSTRACT FROM AUTHOR]

Tin-based perovskite solar cells (T-PSCs) have become the star photovoltaic products in recent years due to their low environmental toxicity and superior photovoltaic performance. However, the easy oxidation of Sn 2+ and the energy level mismatch between the perovskite film and charge transport layer limit its efficiency. In order to regulate the microstructure and photoelectric properties of tin-based perovskite films to enhance the efficiency and stability of T-PSCs, guanidinium bromide (GABr) and organic Lewis-based additive methylamine cyanate (MAOCN) are introduced into the FA 0.9 PEA 0.1 SnI 3 -based perovskite precursor. A series of characterizations show that the interactions between additive molecules and perovskite mutually reconcile to improve the photovoltaic performance of T-PSCs. The introduction of GABr can adjust the band gap of the perovskite film and energy level alignment of T-PSCs. They significantly increase the open-circuit voltage ( V oc ). The MAOCN material can form hydrogen bonds with SnI 2 in the precursor, which can inhibit the oxidation of Sn 2+ ). The synergistic modulation of the dual additives reduces the trap-state density and improves photovoltaic performance, resulting in an increased champion efficiency of 9.34 for 5.22% of the control PSCs. The unencapsulated T-PSCs with GABr and MAOCN dual additives prepared in the optimized process can retain more than 110% of their initial efficiency after aging for 1750 h in a nitrogen glovebox, but the control PSCs maintain only 50% of their initial efficiency kept in the same conditions. This work provides a new perspective to further improve the efficiency and stability of T-PSCs.J sc ). The synergistic modulation of the dual additives reduces the trap-state density and improves photovoltaic performance, resulting in an increased champion efficiency of 9.34 for 5.22% of the control PSCs. The unencapsulated T-PSCs with GABr and MAOCN dual additives prepared in the optimized process can retain more than 110% of their initial efficiency after aging for 1750 h in a nitrogen glovebox, but the control PSCs maintain only 50% of their initial efficiency kept in the same conditions. This work provides a new perspective to further improve the efficiency and stability of T-PSCs.

To promote the solar-energy cascade utilization, it is necessary to increase the thermal effect of irradiation in the catalytic reactions, while simultaneously augmenting the non-thermal effect, so as to fulfill photothermal coupling. Herein, the non-thermal and thermal effect of light radiation on the surface of In 2 O 3 -based catalysts are explored and enhanced by the modification of transition metals Fe and Cu. Optical characterizations combined with water-splitting experiments show that Fe doping greatly broadens the radiation response range and enhances the absorption intensity of semiconductors' intrinsic portion, and Cu doping facilitates the absorption of visible-infrared light. The concurrent incorporation of Fe and Cu offers synergistic benefits, resulting in improved radiation response range, carrier separation and migration, as well as higher photothermal temperature upon photoexcitation. Collectively, these advantages comprehensively enhance the photothermal synergistic water-splitting reactivity. The characterizations under variable temperature conditions have demonstrated that the reaction temperature exerts a significant influence on the process of radiation absorption and conversion, ultimately impacting the non-thermal effect. The results of DFT calculations have revealed that the increasing temperature directly impacts the chemical reaction by reducing the energy barrier associated with the rate-determining step. These findings shine new light on the fundamental mechanisms underlying non-thermal and thermal effect, while also imparting significant insights for photo-thermal-coupled catalyst designing.

Interfacial nonradiative recombination loss is a huge barrier to advance the photovoltaic performance. Here, one effective interfacial defect and carrier dynamics management strategy by synergistic modulation of functional groups and spatial conformation of ammonium salt molecules is proposed. The surface treatment with 3-ammonium propionic acid iodide (3-APAI) does not form 2D perovskite passivation layer while the propylammonium ions and 5-aminopentanoic acid hydroiodide post-treatment lead to the formation of 2D perovskite passivation layers. Due to appropriate alkyl chain length, theoretical and experimental results manifest that COOH and NH 3 + groups in 3-APAI molecules can form coordination bonding with undercoordinated Pb 2+ and ionic bonding and hydrogen bonding with octahedron PbI 6 4- , respectively, which makes both groups be simultaneously firmly anchored on the surface of perovskite films. This will strengthen defect passivation effect and improve interfacial carrier transport and transfer. The synergistic effect of functional groups and spatial conformation confers 3-APAI better defect passivation effect than 2D perovskite layers. The 3-APAI-modified device based on vacuum flash technology achieves an alluring peak efficiency of 24.72% (certified 23.68%), which is among highly efficient devices fabricated without antisolvents. Furthermore, the encapsulated 3-APAI-modified device degrades by less than 4% after 1400 h of continuous one sun illumination., (© 2023 Wiley-VCH GmbH.)

The photocatalytic hydrogen evolution (PHE) offers a promising and sustainable route to fuels and feedstocks from solar energy. Ti 3 C 2 MXene as a highly active and stable earth-abundant material has been employed in photocatalytic hydrogen production due to its excellent conductivity and effective activation of H 2 O molecules. Herein, a synergistic strategy, via introducing atomic-thickness Ti 3 C 2 MXene to tune the defect structure of the ultrathin ZnIn 2 S 4 nanosheets, is reported to improve the PHE activity. By using microstructure characterization and DFT calculation, we reveal the generation of sulfur vacancies (S vac) on the photocatalysts and the improvement of adsorption property for reactant H 2 O molecules at the surface of ultrathin 2D/2D Ti 3 C 2 / S vac -ZnIn 2 S 4 heterojunction. During the reaction, the synergies between sulfur vacancies and Ti 3 C 2 MXene affect the absorption of light, the separation of carriers, and the reaction of H 2 O molecules, thus improving the PHE rate up to 1435.31 μmol·g−1·h−1 with 6.3 times higher than that of S vac -ZnIn 2 S 4 nanosheets (229.16 μmol·g−1·h−1). This work stresses the great importance of synergistic modulation for promoting photocatalytic hydrogen evolution. [Display omitted] [ABSTRACT FROM AUTHOR]

Tin perovskites have received great concern in solar cell research owing to their favorable optoelectronic performance and environmental friendliness. However, due to their poor crystallization and easy oxidation, the performance improvement for tin-based perovskite solar cells (TPSCs) is rather challenging. Herein, reductive 3-hydroxytyramine hydrochloride (DACl) with NH 2 ·HCl and phenol groups as co-additives with SnF 2 is added into the precursor to modulate perovskite crystallization and inhibit Sn 2+ oxidation for high-performance TPSCs. The Lewis base group of NH 2 HCl in DACl could bind to perovskite lattices to modulate the crystallization with suppressed defects in the bulk and grain boundary, whereas reductive phenol groups effectively constrain the Sn 2+ oxidation. Moreover, the undissociated DACl decreases the supersaturated concentration of tin perovskite solution and creates a pre-nucleation site for rapid nucleation to further regulate crystallization. Consequently, the DACl-derived TPSCs achieve a high power-conversion efficiency (PCE) that reaches up to 11%. More impressively, the device remains at 84% of the initial PCE after full-sun illumination in N 2 over 600 h without being encapsulated. This DACl-based synergistic modulation of a lead-free perovskite demonstrates a feasible approach using one molecule with different functional groups to manipulate crystallization, Sn 2+ oxidation, and defect reparation of tin perovskite films, providing a critical guideline for constructing high-quality perovskites by multifunctional additives with high photovoltaic performance.

The article presents a study on the estrogenic activity of single and mixed estrogens when influenced with toxic masking and synergistic modulation from non-estrogenic chemical confounders. It reveals that the non-estrogenic chemicals decrease the estrogenicity of both estrogens. It concludes the consideration of two major challenges in determining the estrogenic activity of complex mixtures which include the designation of estrogenic compounds, and the impact of non-estrogenic toxicants.

[Display omitted] • A facile MoS 2 phase-incorporation strategy for fabricating the highly efficient photocatalysts is proposed. • The in-plane sulfur vacancies induce the transformation of the surrounding 1T-MoS 2 local lattice into a 2H phase. • 2H@1T-MoS 2 phase-incorporation prompts synergistic regulations of both structural and electronic benefits. • ZnIn 2 S 4 @MoS 2 photocatalysts possess rich exposed active sites and high electronic conductivity. • ZnIn 2 S 4 @MoS 2 photocatalysts exhibit high and stable photocatalytic hydrogen evolution. Photocatalytic hydrogen evolution (PHE) is of great significance to pursue sustainable and clean fuel, however, it remains a great challenge due to the high recombination of photo-generated carriers and low efficiency of surface catalytic activity. Here, we discover the synergistic regulations of both structural and electronic benefits by introducing sulfur vacancies in a 1T-MoS 2 nanosheets host to prompt the transformation of the surrounding 1T-MoS 2 local lattice into a 2H phase, leading to the dramatically enhanced PHE activity. Multiple in situ spectroscopic and microscopic characterizations combined with theoretical calculations demonstrated that in-plane sulfur vacancies as active sites can activate the proton, while the 2H@1T-MoS 2 phase-incorporation can effectively regulate the electronic structure and further improve the conductivity. Therefore, the optimized ZnIn 2 S 4 @MoS 2 photocatalyst achieves a high PHE activity of 23,233 μmol g−1 with an apparent quantum yield (AQY) of ∼5.09 %. This work provides a new design for improving the photocatalytic activity by synergistically structural and electronic modulations. [ABSTRACT FROM AUTHOR]

This work applies ternary catalyst design to synergistically modulate the nanostructure and active sites for concurrent, cost-effective and scalable production of hydrogen and formate. The deep mechanistic understanding for the less-explored MFO is useful for the development of bifunctional electrocatalyst towards coupled HER and MFO. [Display omitted] • Ternary electrocatalyst is synthesized for boosting both hydrogen evolution reaction and methanol-to-formate oxidation. • Synergy between WO x and Fe, Ru-based dopants contribute to superior anodic/cathodic activities and durability. • Unique continuous and hierarchical nanostructure benefits to mass transfer and catalyst robustness. • Hydrogen and value-added formate are produced with high FE. • The electrode pair shows high selectivity and durability in alkaline media at large current density. Coupling methanol-to-formate oxidation (MFO) with hydrogen evolution reaction (HER) may promote hydrogen economics by introducing value-added anodic product. Herein, we develop a ternary catalyst Ru&Fe-WO x for boosting both HER and MFO in alkaline media. An electrode pair based on Ru&Fe-WO x delivers 10/100/500 mA/cm2 current density at a low cell-potential of 1.38/1.50/1.62 V with excellent durability and nearly 100 % Faradaic efficiency (FE), outperforming the benchmark pair of Pt/C||RuO 2. By using integrated experimental and theoretical approaches, we verify synergy between WO x host and Ru&Fe-based dopants, which results in optimized H* adsorption on lattice oxygen (HER) as well as enhanced HCOO* desorption on ruthenium site (MFO). In addition, the unique nanostructure of Ru&Fe-WO x may further benefit to the mass transfer and catalyst robustness at large current density. This work thus demonstrates an integrated catalyst design, which is highly efficient for boosting concurrent, cost-effective and scalable production of hydrogen and formate. [ABSTRACT FROM AUTHOR]

Exploring new infrared nonlinear optical (IR NLO) materials with superior overall properties is scientifically and technically important. However, large second-order harmonic generation (SHG) efficiencies and high laser-induced damage thresholds (LIDT) are incompatible, which makes realizing this goal a challenge. The IR NLO performance of an A-N IIB -M IIIA -Q (Q: chalcogen) system was optimized by simultaneously modulating A/(M + N) and M/N ratios (A: alkali metal; N, M: tetra-coordinated metals), and SHG-LIDT balance was achieved. Three new sulfides, KCd 3 Ga 5 S 11 ( 1 ), RbCd 4 Ga 3 S 9 ( 2 ), and Cs 2 Cd 2 Ga 8 S 15 ( 3 ), containing the same CdS 4 and GaS 4 but with different A/(Ga + Cd) and Ga/Cd ratios were obtained. Among these compounds, compound 3 exhibits both the largest SHG efficiency (0.5 × AgGaS 2 ) and LIDT (35 × AgGaS 2 ), which can be ascribed to the Ga/Cd modulation for enhancing the NLO functional motif distortions and SHG efficiency as well as the A/(Ga + Cd) modulation for enlarging the band gap and LIDT. Remarkably, compound 3 is the first phase-matchable IR NLO material in the A-N IIB -M IIIA -Q family. This article proposes a novel avenue to explore infrared nonlinear materials with superior comprehensive properties by modulating the A/(M + N) and M/N ratios.

A simple strategy based on the synergistic modulation of inter-particle and substrate-particle interaction is applied for the large-scale fabrication of two-dimensional (2D) Au and Ag nanoparticle arrays. The surface charge of the substrate is used to redistribute the double layer electric charges on the particles and to modulate the inter-particle distance within the 2D nanoparticle arrays on the substrate. The resultant arrays, with a wide range of inter-particle distances, display tunable plasmonic properties. It can be foreseen that such 2D nanoparticle arrays possess potential applications as multiplexed colorimetric sensors, integrated devices and antennas. Herein, it is demonstrated that these arrays can be employed as wavelength-selective substrates for multiplexed acquisition of surface-enhanced Raman scattering (SERS) spectra. This simple one step process provides an attractive and low cost strategy to produce high quality and large area 2D ordered arrays with tunable properties., (© 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)