Oxygen-ion conductors are central to clean energy technologies. Conventional long-range-ordered oxide-ion conductors require high operating temperatures, which increase cost and limit durability; overcoming the low temperature conductivity gap is a long-standing challenge. We created cerium (Ce)-gadolinium (Gd)-oxygen (O) clusters by thermal-shock exfoliation of fluorite Gd0.1Ce0.9O1.95 and examined their structure and ion transport. These disordered, vacancy-isolated clusters form percolative oxygen-ion pathways without long-range order, delivering exceptional conductivity of 2.14 ± 0.09 siemens per centimeter at 400°C-more than 320-fold higher than most previously reported oxide-ion conductors under comparable conditions. Used as a 0.5 weight % cathode additive in solid oxide fuel cells, they tripled the peak power density to 2.87 ± 0.04 watts per square centimeter at 750°C compared with the pristine Pr0.5Ba0.25Ca0.25CoO3-δ/Gd0.1Ce0.9O1.95 cathode and reversed degradation from -13.2 to +3.4% per 100 hours. These findings overturn the paradigm that high oxygen-ion conductivity requires long-range order and highlight Ce-Gd-O clusters as enablers for advanced energy technologies.
ABSTRACT Dynamic afterglow carbon dots (CDs) materials, capable of long‐duration emission and dynamic color changes after excitation, hold promise for widespread applications in high‐level encryption and visual sensing. However, the single‐variable response afterglow color changing limits the potential of CDs for multidimensional information encoding and dynamic encryption in complex environments. Here, we report metal‐free CDs with triple‐variable responses (time, temperature, and excitation wavelength) for multiple dynamic afterglow colors and an ultra‐high afterglow brightness (406 cd m −2 ) far exceeding those of other afterglow materials. Based on the synergistic effect of triple matrix confinement and interface effects, room‑temperature phosphorescence (RTP) and thermally activated delayed fluorescence (TADF) are integrated into a single CD system. Owing to the different lifetimes of the dual‐mode afterglow (phosphorescence and TADF) and their varying sensitivities to temperature and excitation wavelength, time‐dependent afterglow colors (TDAC), excitation‐dependent afterglow colors (EDAC), and thermochromic afterglow (TCAG) are simultaneously achieved. Finally, we also designed a three‐dimensional variable‐response color code that varies with time, temperature, and excitation wavelength, spanning the entire visible spectrum. This platform enables high‐capacity, programmable, full‐gamut, and visually intuitive information encryption and display, providing a promising pathway for advanced, multidimensional anti‐counterfeiting and secure communication technologies.
Phosphorescent materials that exhibit high efficiency and intensity are crucial for practical applications. In this study, we devised a novel strategy to enhance carbon dots (CDs) phosphorescence based on a crosslink-enhanced emission (CEE) and layer-by-layer self-assembly (LBL) synergistic enhancement design. The seed CDs are initially functionalized with cationic polymers on their surfaces, followed by assembly with negatively charged matrices to enhance their phosphorescence. This leads to a significant phosphorescence intensity enhancement by a factor of more than 88, enabling visual readability even in bright fields. Their lifetime is prolonged from 0.13 to 0.41 s and the maximum phosphorescence quantum yield reached up to 27.2 %. Detailed investigations revealed that CEE and LBL significantly inhibited molecular vibrations and protected the triplet excitons of CDs from oxygen quenching, enhancing phosphorescence emission. The loading capacity of the CDs in the matrix was significantly enhanced owing to the uniform dispersion induced by the electrostatic interactions between CDs and the substrate. Furthermore, we envision potential applications of these CDs for anti-counterfeiting and crack detection in bright fields.
Phenolic compounds stand as consequential chemical precursors, boasting an extensive array of industrial applications. The worldwide yield of such compounds attained 17 million tons annually, and a substantial volume of effluent characterized by elevated phenolics content along with inorganic salinity was emanated from the manufacturing processes, which would exert profound deleterious impacts upon the ecosystem and aquatic environment. Scant literature was available regarding efficacious treatment of these high-salinity phenolic wastewaters and complete recovery of its constituents currently. In this study, initially, various high-salinity phenolic wastewaters were treated in bipolar membrane electrodialysis (BMED) system, and the migration behavior of constituents was investigated. Drawing upon the migration patterns and the efficacy of BMED, a closed-loop integrated process of BMED and resin adsorption was proposed to thoroughly address this kind of wastewater and attain comprehensive material reclamation. Because of the wide use of salicylic acid (SA) all over the world, the enormous production in China, and the complexity of the sewage which contained rich Na2SO4, phenol, and SA from manufacturing process, SA manufacturing wastewater was selected as the representative sample. For the BMED process, the desalination rate got 99.4 % under the optimum conditions. The concentrations of H2SO4 and NaOH obtained were 0.56 and 0.78 mol/L. The preliminary separation of phenol and SA was realized during desalination. Then, the effluent of BMED feed compartment was injected into two-stage resin unit. The satisfactory regeneration of both spent resins was achieved, and high-purity phenol and SA were obtained. No contaminants were undetected in the effluent, allowing for the reuse of the effluent within BMED. The complete resource utilization of SA manufacturing wastewater was realized, indicating the viability of proposed integrated process for treating and resource recovering of analogous high-salinity industrial phenolic wastewater.
We present GenN2N, a unified NeRF-to-NeRF translation framework for various NeRF translation tasks such as text-driven NeRF editing, colorization, super-resolution, in-painting, etc. Unlike previous methods designed for individual translation tasks with task-specific schemes, GenN2N achieves all these NeRF editing tasks by employing a plug-and-play image-to-image translator to perform editing in the 2D domain and lifting 2D edits into the 3D NeRF space. Since the 3D consistency of 2D edits may not be assured, we propose to model the distribution of the underlying 3D edits through a generative model that can cover all possible edited NeRFs. To model the distribution of 3D edited NeRFs from 2D edited images, we carefully design a VAE-GAN that encodes images while decoding NeRFs. The latent space is trained to align with a Gaussian distribution and the NeRFs are supervised through an adversarial loss on its renderings. To ensure the latent code does not depend on 2D viewpoints but truly reflects the 3D edits, we also regularize the latent code through a contrastive learning scheme. Extensive experiments on various editing tasks show GenN2N, as a universal framework, performs as well or better than task-specific specialists while possessing flexible generative power. More results on our project page: https://xiangyueliu.github.io/GenN2N/.
Precise detection of zinc ion is of fundamental importance in the fields of environment protection and food safety. A comprehensive understanding of the sensing mechanism will help to the design of such sensors. The detailed photophysical process of a zinc ion sensor as well as the sensing mechanism are uncovered with the aid of density functional theory (DFT) and time-dependent density functional theory (TDDFT). Both the ground state and first excited state potential energy surfaces (PES) of the sensor are carefully explored to reveal the photo-physical process of the sensor. Excited state intramolecular proton transfer (ESIPT) is observed on the S1 state PES. Then, the twist motion of C=N double bond is triggered after the ESIPT process, which leads to a twisted intramolecular charge transfer (TICT) state. This TICT state is found to make the sensor non-emissive. With the addition of Zn2+, the TICT state is eliminated which greatly enhances the fluorescence of the sensor and achieves zinc ion detection. The interaction of the sensor with Cd2+ and Hg2+ are also explored, which well explains the good selectivity of the sensor.
Carbonized polymer dots (CPDs) with white-light-emitting property have greatly promising application in next generation of lighting and display technologies. However, most of the reported CPD materials exhibit single peak emission and narrow emission band, resulting in difficulty to obtain white-light emission. In this work, the ultrabroadband triple-peak emission (red, green, and blue) CD-based materials with high-efficiency white lightemitting property are realized for the first time by the Forster resonance energy transfer (FRET). Blue and green emissions are derived from the fluorescence and phosphorescence of donor CPDs, while the red light is derived from receptor by FRET. Remarkably, the fabricated CPD materials show bright pure white-light emission with high overall quantum yield (QY) of 36% and the full width at half maximum of 235 nm. Besides, afterglow colors of CPD-based materials can be tuned from green to red by adjusting the ratio of donor and acceptor. Based on the high-efficiency and wide-spectrum pure white light emission characteristics of CPD-based composites, white light emitting diodes were fabricated and they exhibit bright warm white light with CIE and CCT of (0.35, 0.31) and 4041 K.
Multicolor afterglow patterns with transparent and traceless features are important for the exploration of new functionalities and applications. Herein, we report a direct in situ patterning technique for fabricating afterglow carbon dots (CDs) based on laser direct writing (LDW) for the first time. We explore a facile step-scanning method that reduces the heat-affected zone and avoids uneven heating, thus producing a fine-resolution afterglow CD pattern with a minimum line width of 80 μm. Unlike previous LDW-induced luminescence patterns, the patterned CD films are traceless and transparent, which is mainly attributed to a uniform heat distribution and gentle temperature rise process. Interestingly, by regulating the laser parameters and CD precursors, an increased carbonization and oxidation degree of CDs could be obtained, thus enabling time-dependent, tunable afterglow colors from blue to red. In addition, we demonstrate their potential applications in the in situ fabrication of flexible and stretchable optoelectronics.
Achieving a stimulus-responsive, multi-colour, long-lived luminescence based on single-emissive-center carbon dots (CDs) is highly desirable for numerous promising applications. However, the fabrication of such materials remains a formidable challenge because of the limited paths of exciton transfer. Herein, we report a facile strategy to achieve a colour-tuneable afterglow by selectively activating different exciton transfer channels in a carbon dot-cyanuric acid (CA) composite (CD@CA) by alkali induction. Upon alkali treatment, CD@CA exhibited a noticeable afterglow colour change from cyan to yellow with an excellent reversible pH response. Remarkably, the yellow afterglow efficiency is as high as 34.8% and its average lifetime can reach 0.535 s. Detailed analyses revealed the existence of two exciton transport pathways within the system. Excitons can be transduced from CA to CDs via F & ouml;rster resonant energy transfer, leading to a cyan afterglow. In an alkaline environment, this channel was destroyed, and the inherent phosphorescence exciton transport channel of CDs was simultaneously activated and enhanced. Alkali-induced CD ionization and the formation of rigid crystal networks boost intersystem crossing rates and reduce non-radiative transitions, resulting in a bright yellow afterglow. Furthermore, based on the colour-tuneable afterglow properties of the system, we illustrated the potential applications of CD@CA in advanced information encryption. This study provides guidance in the development of multi-colour afterglow materials with stimulus-responsive characteristics to meet the growing demand for highly secure information storage materials. Achieving a colour-tuneable afterglow by selectively activating different exciton transfer channels in a carbon dot-cyanuric acid composite by alkali induction.
Low-temperature direct ammonia fuel cells (DAFCs) use carbon-neutral ammonia as a fuel, which has attracted increasing attention recently due to ammonia's low source-to-tank energy cost, easy transport and storage, and wide availability. However, current DAFC technologies are greatly limited by the kinetically sluggish ammonia oxidation reaction (AOR) at the anode. Herein, we report an AOR catalyst, in which ternary PtIrZn nanoparticles with an average size of 2.3 ± 0.2 nm were highly dispersed on a binary composite support comprising cerium oxide (CeO 2 ) and zeolitic imidazolate framework-8 (ZIF-8)-derived carbon (PtIrZn/CeO 2 -ZIF-8) through a sonochemical-assisted synthesis method. The PtIrZn alloy, with the aid of abundant OH ad provided by CeO 2 and uniform particle dispersibility contributed by porous ZIF-8 carbon (surface area: ∼600 m 2 g −1 ), has shown highly efficient catalytic activity for the AOR in alkaline media, superior to that of commercial PtIr/C. The rotating disk electrode (RDE) results indicate a lower onset potential (0.35 vs. 0.43 V), relative to the reversible hydrogen electrode at room temperature, and a decreased activation energy (∼36.7 vs. 50.8 kJ mol −1 ) relative to the PtIr/C catalyst. Notably, the PtIrZn/CeO 2 -ZIF-8 catalyst was assembled with a high-performance hydroxide anion-exchange membrane to fabricate an alkaline DAFC, reaching a peak power density of 91 mW cm −2 . Unlike in aqueous electrolytes, supports play a critical role in improving uniform ionomer distribution and mass transport in the anode. PtIrZn nanoparticles on silicon dioxide (SiO 2 ) integrated with carboxyl-functionalized carbon nanotubes (CNT–COOH) were further studied as the anode in a DAFC. A significantly enhanced peak power density of 314 mW cm −2 was achieved. Density functional theory calculations elucidated that Zn atoms in the PtIr alloy can reduce the theoretical limiting potential of *NH 2 dehydrogenation to *NH by ∼0.1 V, which can be attributed to a Zn-modulated upshift of the Pt–Ir d-band that facilitates the N–H bond breakage.
The selective separation and purification of ART and ARE using molecularly imprinted membrane (MIM) has attracted considerable attention, but most of con-ventional blending MIM face low adsorption capacity and poor selectivity due to the blockage of imprinting sites. Herein, an alternative ART imprinted MnO2 nanowires "coating" membrane (MINM) with hydrophilicity was fabricated by vacuum filtration of imprinted MnO2 nanowires and graphene oxide nanosheets on PVDF membrane surface for selective ART separation. For the MINM, the imprinted MnO2 nanowires coating offers more available exposed imprinting sites on the MINM surface compared to that of the blending MIM, while the introduction of graphene oxide improves the hydrophilicity of MINM, significantly reducing the non-specific absorption. Consequently, the MINM exhibits ultrahigh ART adsorption capacity and selectivity, with the ART adsorption amount of 335 mg g(-1) at 5 min using dynamic cross-flow separation system, about 12.18 times higher than that of ARE (27.5 mg g(-1)), and the separation factor (a) value of 12.39. Moreover, the ATR FT-IR dynamic spectrum discloses the in-situ formation of H-bond between ART and MINM, playing a key role in the selective adsorption process. This work provides an alternative strategy to prepare "coating" MIM for high-efficient and selective separation of complex analogue systems.
Generally, 2D "thin-film" structural molecularly imprinted membranes (MIMs) prepared by the common phase inversion method suffer low adsorption capacity due to the easy embedment of imprinting sites. Herein, an alternative "delayed phase inversion" strategy was first developed to construct a natural loofah-based 3D porous MIM (LPMIM), in which the as-prepared molecularly imprinted polymers (MIPs) with artesunate (ARU) as dummy template spontaneously interacted with the polyvinylidene fluoride (PVDF) pre-treated loofah framework (LPM), and evenly anchored on loofah fiber surfaces, similar to the cobweb locking raindrops. Interestingly, the natural 3D fiber cross networks of loofah not only provided sufficient capacity and space to support MIPs without causing aggregation and maintains high flux, but also the inherent high mechanical strength of loofah fibers endowed the LPMIM with excellent stability. Under dynamic conditions the ART adsorption capacity of LPMIM could be further remarkably improved by tailoring the flow rate of 1.19 mL·cm−2·min−1, up to 334.70 mg/g. As a result, effective enhancement in the artemisinin (ART) adsorption capacity were achieved for the LPMIM, which was about 2.25 times higher than that of the common blend MIM prepared by common phase inversion method (148.30 mg/g). Moreover, the LPMIM possessed high ART selectivity towards its analogue, artemether (ARE), giving an ART/ARE ratio of 2.7. Furthermore, the LPMIM displayed excellent recycling performance. By altering the template of MIPs, the corresponding LPMIM can be expanded to highly selective separation of other substrates along with large absorption capacity. This work highlights a universal strategy to construct novel MIMs with high absorption capacity and selectivity using bio-based fiber cross frameworks.
In this work, a simple metal-organic framework (MOF) material, UiO-66-NH2, was prepared for the highly efficient separation of artemisinin (Art) and artesunate (Aru). Selective adsorption tests showed that UiO-66-NH2 presented a much higher selectivity toward Aru than Art (alpha(Aru/Art) = 40.74). The N-2 adsorption-desorption isotherm results of UiO-66-NH2 indicated a suitable pore size to enable the free entry of Art and Aru. Contact angle analysis indicated that UiO-66-NH2 is hydrophilic with the-NH2 group, and can interact with the hydrophobic Aru through hydrogen bonding between the-NH2 and-COOH groups, which is not possible with the hydrophobic Art. The selective adsorption of Aru onto UiO-66-NH2 may be attributed to three factors: pore size, functional groups, and difference in hydrophobic/hydrophilic characteristics between the adsorbent and adsorbate. Molecularly imprinted polymers (MIPs) were prepared using Aru as a template for selective adsorption experiments to verify the excellent selectivity of UiO-66-NH2. The adsorption amount (65.24 mg g(-1)) and selectivity factor (alpha(Aru/Art) = 40.74) of UiO-66-NH2 toward Aru were significantly better than those of the MIPs (2.039 mg g(-1) and 3.072, respectively). The binding capacity and better selectivity of UiO-66-NH2 provide evidence supporting the potential of MOF adsorbents for the separation of various analogous molecules.
The production of H(2)O(2 )through photocatalysis is a green and economical alternative to conventional methods. Here, we prepared poly (heptazine imide) (PHI) phase polymeric carbon nitrides (Li-PCN) by facile lithium ions -assistant post-condensation method. Lithium ions not only can optimize condensation process, but also exfoliate and tailor PCN, resulting in higher crystallinity, excellent photo-absorption range, which enhance surface adsorption of dioxygen, and increase the number of electron transfers in the reaction. Based on the above ad-vantages, the Li-PCN exhibits excellent photocatalytic H2O2 (2680 mu mol g -1h- 1) production activity under visible light, which was about 35.7 times higher than that of PCN. Besides, we have increased the concentration of H(2)O(2 )through changing reaction solution to a final content of 4.8613 mM. Furtherly, the homemade H(2)O(2 )production was used to degrade methyl orange pollution by Fenton reaction. This work provides a new synthetic route to PHI and highlights the function of lithium ions, which can promote the development of more efficient photo -catalysts for H(2)O(2 )production.
Hydrogen fuel cells currently rely on expensive platinum group metal nanoparticle catalysts [1]. For green hydrogen production and utilization to become widely commercially viable, the cost of the devices that produce and utilize hydrogen must be significantly reduced. Platinum group metal-free (PGM-free) catalysts have the potential to greatly reduce this cost, and materials consisting of single transition metal atoms embedded in a nitrogen-doped graphitic carbon structure have shown particular promise for use as fuel cell cathodes [2]. A better understanding of the active site properties in these materials is still needed, however, to improve their stability and design new active site structures with enhanced properties [3]. Due to the atomic-scale nature of the active sites in these materials, scanning transmission electron microscopy (STEM) and electron energy-loss spectroscopy (EELS) have proven invaluable for demonstrating their atomically dispersed nature and composition [4]. Conventional STEM techniques have limited ability to correlate the local bonding environment and oxidation state of the metal atoms, for example, or track changes in the catalyst structure both during synthesis and as a result of cycling, which would provide a deeper understanding of the relationship between active site and catalyst properties. Here, we demonstrate advanced electron microscopy techniques that provide both enhanced and previously inaccessible information about PGM-free catalysts and their active sites. We show developments in automated identification of metal atom positions, which we use both to generate statistics about interatomic distances and to automatically position the STEM probe on individual atoms for EELS data acquisition. The former allows information about the presence of dual-metal site structures to be extracted, for example, and the latter allows compositional information with improved SNR to be obtained. Rapid automatic probe positioning also presents the opportunity for measuring the effect of local bonding environment on metal atom oxidation state, which cannot be obtained manually since these sites are typically unstable under the beam. In addition, we will show identical-location STEM (IL-STEM) techniques that allow the evolution of catalyst morphology and properties to be tracked at high resolution across synthesis steps and accelerated stress tests [5]. In particular, we use IL-STEM imaging and EELS to track deposition of graphitic material on the surface of a PGM-free catalyst that significantly improves the material’s durability, as well as track the change in the nanoscale graphitic carbon structure of the material as a function of electrochemical cycling. By providing access to enhanced compositional and bonding state information, as well as the ability to track properties as a material evolves, these techniques will advance our knowledge of PGM-free catalysts and enable better control over their properties in the future, accelerating wide-spread use of hydrogen fuel cells [6]. References: [1] D.A. Cullen et al., Nat. Energy 6 , 462 (2021). [2] G. Wu, Front. Energy 11 , 286 (2017). [3] U. Martinez et al., Adv. Mater. 31 , 1806545 (2019). [4] H.T. Chung et al., Science 357 , 479 (2017). [5] H. Yu et al., ACS Appl. Mater. Interfaces (2022). [6] This work was supported by the U.S. Department of Energy, Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office under the Electrocatalysis (ElectroCat) consortium. Electron microscopy research was supported by the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory.
Replacing Pt-based catalysts with metal-organic frameworks (MOFs) derived single-atom catalysts (SACs) for oxygen reduction reaction (ORR) has largely been impeded by the hidden activity of SACs due to the challenges in exposing unactivated sites and regulating their electronic states. Here we demonstrate the synthesis of highly exposed iron single atoms and clusters on imidazole frameworks derived carbon (scCO(2)-FeC@FeNC) by super-critical CO2 (scCO(2)) assisted strategy. The scCO(2) fluid not only incises dodecahedron into uniform cubes with tenth of thickness but also constructs hierarchical pores in frameworks without utilization of templates, and thus in favor to exposure of inactive sites. Moreover, theoretical simulations disclose that the adjacent cluster weakens hybridization between occupied d-orbitals of iron for Fe-N moiety and p-orbitals of adsorbed oxygen, thereby optimizing adsorption-desorption process of oxygenated intermediates and accelerating ORR kinetics. With these merits, scCO(2)-FeC@FeNC delivers an ORR activity with half-wave potential of 0.91 V in alkaline solution. The Zn-air battery using scCO(2)-FeC@FeNC as air cathode has a specific capacity of 784.1 mAh gZn(-1) and long-time durability of 200 h, surpassing commercial Pt/C-based Zn-air battery. This work provides a promising approach to fabricate MOF-derived metal-N-C ORR electrocatalysts with high performance.
Ammonia (NH3) has proved to be an effective alternative to hydrogen in low-temperature fuel cells via its direct ammonia oxidation reaction (AOR)(1). However, the kinetically sluggish AOR has prohibitively hindered the attractive direct ammonia fuel cell (DAFC) applications. Here, we report an efficient AOR catalyst, in which ternary PtIrM (M: Ni or Zn) alloy nanoparticles well dispersed on a binary composite support consisting of porous silicon dioxide (SiO2) and carboxyl-functionalized carbon nanotube (PtIrNi/SiO2-CNT-COOH) through a sonochemical-assisted synthesis method (2). The PtIrNi alloy nanoparticles, with the aid of abundant OHad provided by porous SiO2 and the improved electrical conductivity by CNTs, exhibit remarkable catalytic activity for the AOR in alkaline media. It is evidenced by a lower onset potential (∼0.40 V vs reversible hydrogen electrode (RHE)) at room temperature than that of commercial PtIr/C (ca. 0.43 V vs RHE). Increasing NH3 concentrations and operation temperatures can significantly enhance AOR activity of this PtIrNi nanoparticle catalyst. Specifically, the catalyst at the temperature of 80 °C exhibits a much lower onset potential (∼0.32 V vs RHE) and a higher peak current density, indicating that DAFCs operated at a higher temperature are favorable for increased performance. References (1) Adli, N. M.; Zhang, H.; Mukherjee, S.; Wu, G., Review—Ammonia Oxidation Electrocatalysis for Hydrogen Generation and Fuel Cells. Journal of The Electrochemical Society 2018, 165 (15), J3130-J3147. (2) Li, Y.; Li, X.; Pillai, H. S.; Lattimer, J.; Mohd Adli, N.; Karakalos, S.; Chen, M.; Guo, L.; Xu, H.; Yang, J.; Su, D.; Xin, H.; Wu, G., Ternary PtIrNi Catalysts for Efficient Electrochemical Ammonia Oxidation. ACS Catalysis 2020, 10 (7), 3945-3957.
Ammonia (NH3) has proven to be a cost-effective alternative to hydrogen for powering fuel cells via its direct oxidation to nitrogen and water. However, sluggish kinetics of the ammonia oxidation reaction (AOR) have greatly hindered the commercial application of direct ammonia fuel cells (DAFCs). Here we report an efficient AOR catalyst that consists of PtIrNi alloy nanoparticles anchored on a binary support of porous silicon dioxide and carboxyl-functionalized carbon nanotubes (PtIrNi/SiO2-CNT-COOH) through a sonochemical-assisted synthesis strategy. The PtIrNi alloy nanoparticles, with the aid of abundant OHad provided by porous SiO2, and the improved electronic conductivity contributed by CNT, exhibit remarkable catalytic activity for the AOR in alkaline media, with a lower onset potential (~0.40 V vs. RHE) at room temperature, than that of commercial PtIr/C (~0.43 V vs. RHE). Constant-potential density functional theory (DFT) calculations showed that the Pt-Ir ensembles on {100}-terminated surfaces serve as the active site, the introduction of Ni to which raises the center energy of the density of states projected onto the group d-orbitals and thus lowers the theoretical onset potential for *NH2 dehydrogenation to *NH when compared to Pt and Pt3Ir alloy. Varying the NH3 concentration and operation temperature shows a significant influence on the AOR performance of this catalyst. Specifically, AOR activity of the optimal PtIrNi nanoparticle catalyst can be significantly enhanced by elevating the temperature to 80ºC, with a much lower onset potential (~0.32 V vs. RHE), indicating that DAFC can be operated at higher temperature for increased performance.
The rapid development of flexible and wearable electronics proposes the persistent requirements of high‐performance flexible batteries. Much progress has been achieved recently, but how to obtain remarkable flexibility and high energy density simultaneously remains a great challenge. Here, a facile and scalable approach to fabricate spine‐like flexible lithium‐ion batteries is reported. A thick, rigid segment to store energy through winding the electrodes corresponds to the vertebra of animals, while a thin, unwound, and flexible part acts as marrow to interconnect all vertebra‐like stacks together, providing excellent flexibility for the whole battery. As the volume of the rigid electrode part is significantly larger than the flexible interconnection, the energy density of such a flexible battery can be over 85% of that in conventional packing. A nonoptimized flexible cell with an energy density of 242 Wh L −1 is demonstrated with packaging considered, which is 86.1% of a standard prismatic cell using the same components. The cell also successfully survives a harsh dynamic mechanical load test due to this rational bioinspired design. Mechanical simulation results uncover the underlying mechanism: the maximum strain in the reported design (≈0.08%) is markedly smaller than traditional stacked cells (≈1.1%). This new approach offers great promise for applications in flexible devices.
Photocatalytic degradation is an effective method for fast removal of dye‐contaminated water. In the present work, a bismuth oxide/zinc sulfide‐cellulose acetate photocatalytic membrane (Bi2O3/ZnS‐CA) is successfully fabricated via the phase‐inversion method with a Bi2O3/ZnS heterojunction as the photocatalyst. The Bi2O3/ZnS‐CA membranes shows high photocatalytic activity in degradation of Rhodamine B (RhB) under visible‐light irradiation due to the Bi2O3/ZnS heterojunction structure contributing to the high efficiency of photogenerated charge separation. The photodegradation efficiency of Bi2O3/ZnS‐CA membrane is significantly enhanced (about 30% improvement) and the photodegradation kinetic is four times faster than that of the Bi2O3‐CA and the ZnS‐CA membranes. Moreover, the Bi2O3/ZnS‐CA membrane exhibits excellent permeation flux (649.7 L m−2 h−1) and high porosity (69.94%). The Bi2O3/ZnS‐CA membrane also shows good adsorption performance of RhB, which could enhance the interaction between RhB and the catalyst. This work provides a new sight to construct highly effective visible‐light‐driven photocatalytic membranes for continuous organic dye treatment.