Search

Nonlinear nanophotonic devices have brought about great advances in the fields of nano-optics, quantum science, biomedical engineering, etc. However, in order to push these nanophotonic devices out of laboratory, it is still highly necessary to improve their efficiency. Since obtaining novel nanomaterials with large nonlinearity is of crucial importance for improving the efficiency of nonlinear nanodevices, we propose the two-dimensional (2D) perovskites. Different from most previous studies which focused on the 2D perovskites in large scale (such as the bulk materials or the thick flakes), herein we studied the 2D perovskites nanosheets with thickness of ∼50 nm. The high-order nonlinear processes including multi-photon photoluminescence and third-harmonic generation (THG) have been systematically investigated, and it is found the THG process can have a high conversion efficiency up to ∼8 × 10−6. Also, it is observed that the nonlinear responses of 2D perovskites have large optical anisotropy, i.e., the polarization ratio for the incident polarization dependence of nonlinear response can be as high as ∼0.99, which is an impressive record in the perovskite systems. Our findings reveal the properties of high efficiency and huge optical anisotropy in the nonlinear processes of 2D perovskite nanosheets, shedding light on the design of advanced integrated nonlinear nanodevices in future.

Photocatalysis and electrocatalysis have emerged as promising technologies for addressing the energy crisis and environmental issues. However, the widespread application of these technologies is hampered by the challenge of scaling up the production of photo/electrocatalysts that are not only highly active and stable but also cost‐effective and environmentally benign. This review delves into the latest advancements in the large‐scale synthesis of photo/electrocatalysts. The factors to be considered in the large‐scale production of catalysts are discussed first. The synthesis methods for batch preparation of photo/electrocatalysts are then comprehensively introduced, with a thorough discussion of their respective advantages and limitations. Moreover, the data analysis via machine learning techniques, which not only accelerates the identification and refinement of potential new catalysts but also offers insights for enhancing the high‐throughput synthesis of catalysts, is introduced in detail. Then the representative examples are presented to illustrate the applications of large‐scale catalysts in the field of industrial‐level photo/electrocatalysis. Finally, the challenges and prospects in the development of large‐scale production of photo/electrocatalysts are discussed. By bridging the gap between laboratory research and industrial application, this review aims to provide a reference for the future of large‐scale preparation of photo/electrocatalysts in sustainable energy conversion and beyond. [ABSTRACT FROM AUTHOR]

Structural adhesives that do not require heating are in high demand in the automotive and electronics industries. However, it remains a challenge to develop robust adhesives that rapidly achieve super adhesion near ambient temperature. Herein, a room‐temperature curable, fast‐bonding, and super strong epoxy‐based structural adhesive was designed from the perspective of cross‐scale structure, which lies in threefold pivotal aspects: (i) high branching topology of glycerol carbonate‐capped polyurethane (PUGC) increases the kinetics of the ring‐opening reaction, contributing to fast crosslinking and the formation of abundant urethane and hydroxyl moieties; (ii) asynchronous crosslinking of epoxy and PUGC synergistically induces phase separation of PUGC within the epoxy resin and the resulting PUGC domains surrounded by interpenetrated shell serves to efficiently toughen the matrix; (iii) abundant dynamic hydrogen bonds including urethane and hydroxyl moieties, along with the elastomeric PUGC domains, dissipate energy of shearing force. As a result, the adhesive strength rapidly grows to 16 MPa within 4 hours, leveling off to 21 MPa after 7 hours, substantially outperforming commercial room‐temperature curable epoxy adhesives. The results of this study could advance the field of high‐performance adhesives and provide valuable insights into designing materials for efficient curing at room temperature. [ABSTRACT FROM AUTHOR]

The implementation of hot melt adhesives reaching structural adhesion with both impact resistance and detachability is of prospective industry value but still remains challenging. In this work, 2‐amino‐4‐hydroxy‐6‐methylpyrimidine serving as both chain extender and end‐capping reagent due to its isomerism, was developed to construct a supramolecular polyurethane‐derived hot melt structural adhesive. The as‐synthesized PUM elastomers occurs obvious decrease of molecular weight at 80°C compared to room temperature, revealing the existence of self‐complementary 2‐ureido‐4[1H]‐pyrimidinone (UPy) motifs at chain ends. This unique structure allows to chemically incorporate abundant hierarchical and quadruple hydrogen bonding moieties, which results in remarkable enhancement of shear strength, ranging from 6.4 to 16.6 MPa. More importantly, it also exhibits unique impact‐strengthening and reproducible adhering ability. The Hopkinson‐press‐bar and cyclic tensile tests manifest that quadruple hydrogen bonds play a pivotal role in buffering external forces and increasing energy dissipation when exposed to high velocity impacts. The true stress and strain synchronously increase as the strain rate augments while the shear strength can even roar up to ~18 MPa at high tensile speed. With regard to mild synthetic conditions, atomic economic use of reactants, it is promising that this material has industrial potential to be utilized in applications referred to energy‐absorption and reproducible structural adhesion. [ABSTRACT FROM AUTHOR]

Developing chiral electrode catalysts for enantioselective electrosynthesis is a great challenge, as it requires catalysts that possess both high activity and enantioselectivity. Precise synthesis of nanoclusters and single atoms coexisting chiral catalysts provide a promising pathway for enhancing asymmetric catalytic performance. Herein, chiral electrode catalysts are fabricated comprising gold clusters (R‐AuC) and single atoms (R‐AuS) on graphene oxide (R‐AuC/S@GO) through an assembly‐irradiation strategy. Thereinto, the R‐Aus is in situ generated from R‐AuC under light irradiation. The monoatomization process can be precisely regulated by changing the wavelength of the light, resulting in four Au‐based chiral electrode (R‐Au@GO) catalysts with different ratios of nanoclusters and single atoms. These chiral electrodes are applied in the electrocatalytic enantioselective hydrogenation of methyl benzoylformate (MB) to chiral methyl mandelate (S‐MM), and the R‐AuC/S‐2@GO with ≈26% R‐AuC and 74% R‐AuS achieve the highest catalytic activity (35 µmol cm−2 h−1 productivity) and enantioselectivity [97% enantiomeric excess (ee)]. Detailed experimental analysis and density functional theory calculations reveal that the R‐AuS on GO promotes the in situ generation of H* species, and R‐AuC mainly drives the enantioselective conversion of MB by transferring the H* species to the carbonyl group of MB, ultimately yielding chiral S‐MM. [ABSTRACT FROM AUTHOR]

Near‐infrared light‐driven photocatalytic CO2 reduction (NIR‐CO2PR) holds tremendous promise for the production of valuable commodity chemicals and fuels. However, designing photocatalysts capable of reducing CO2 with low energy NIR photons remains challenging. Herein, a novel NIR‐driven photocatalyst comprising an anionic Ru complex intercalated between NiAl‐layered double hydroxide nanosheets (NiAl‐Ru‐LDH) is shown to deliver efficient CO2 photoreduction (0.887 μmol h−1) with CO selectivity of 84.81 % under 1200 nm illumination and excellent stability over 50 testing cycles. This remarkable performance results from the intercalated Ru complex lowering the LDH band gap (0.98 eV) via a compression‐related charge redistribution phenomenon. Furthermore, transient absorption spectroscopy data verified light‐induced electron transfer from the Ru complex towards the LDH sheets, increasing the availability of electrons to drive CO2PR. The presence of hydroxyl defects in the LDH sheets promotes the adsorption of CO2 molecules and lowers the energy barriers for NIR‐CO2PR to CO. To our knowledge, this is one of the first reports of NIR‐CO2PR at wavelengths up to 1200 nm in LDH‐based photocatalyst systems. [ABSTRACT FROM AUTHOR]

The traditional rearview mirror method cannot fully guarantee safety when driving trucks. RGB and infrared images collected by cameras are used for registration and recognition, so as to achieve the perception of surroundings and ensure safe driving. The traditional scale-invariant feature transform (SIFT) algorithm has a mismatching rate, and the YOLO algorithm has an optimization space in feature extraction. To address these issues, this paper proposes a truck surround sensing technique based on multi-features and an improved YOLOv5 algorithm. Firstly, the edge corner points and infrared features of the preset target region are extracted, and then a feature point set containing the improved SIFT algorithm is generated for registration. Finally, the YOLOv5 algorithm is improved by fusing infrared features and introducing a composite prediction mechanism at the prediction end. The simulation results show that, on average, the image stitching accuracy is improved by 17%, the time is reduced by 89%, and the target recognition accuracy is improved by 2.86%. The experimental results show that this method can effectively perceive the surroundings of trucks, accurately identify targets, and reduce the missed alarm rate and false alarm rate. [ABSTRACT FROM AUTHOR]

This study conducts hydrothermal leaching of commercial LiFePO4 (LFPO) cathode materials with oxalic acid, citric acid, or glycine without any other oxidants or reductants. Of these acids, glycine exhibits the weakest leaching behavior, with the leaching efficiency of lithium (Li), iron (Fe), or phosphorus (P) less than 15% even at 200 °C and an acid concentration of 0.8 mol L−1 for 10 min. For oxalic acid, at 200 °C for 10 min, with a pulp density of 30 g L−1 and an acid concentration of 0.8 mol L−1, the leaching efficiencies for Li and P are 100% and 97%, respectively, and 98.5% of Fe precipitates as iron oxalate (FeC2O4) that can be used as a precursor for preparing LFPO cathode materials. Citric acid shows the highest leaching efficiency for Li, Fe, and P, reaching 96%, 100%, and 88%, respectively, at 90 °C for 10 min with a pulp density of 10 g L−1 and an acid concentration of 0.8 mol L−1. The continuous hydrothermal leaching of LFPO cathode materials with citric acid is first achieved. These results clarify the superiority of citric acid over oxalic acid and glycine with respect to the leaching efficiency for Li, Fe, and P from LFPO batteries under hydrothermal conditions. [ABSTRACT FROM AUTHOR]

Conventional adhesives often emit volatile organic compounds (VOCs), which have a negative impact on human health. In this paper, an environmentally‐friendly supramolecular adhesive PD which has high adhesive and low VOCs emission is prepared by the reaction between polyethyleneimine (PEI) and 3,4‐dihydroxybenzaldehyde (DBA). PD containing abundant catechol groups exhibit excellent adhesion to wood substrates and is able to reach a maximum shear strength of 5.20 ± 0.39 MPa. One factor is attributed to multiple reactions between PEI, and DBA and oxidation of DBA. These reactions construct a complex three‐dimensional cross‐linked structure which is very helpful to improve the bonding performance of the adhesive. Another reason refers to the fact that a large number of catechol groups in PD can form a lot of hydrogen bonds with the amino group in PEI and the hydroxyl group in the wood substrate. These hydrogen bonds play an important role in enhancing shear strength. PD adhesives have a stronger bond strength than commercial chloroprene rubber (CR, Pattex‐PXL) and polyvinyl acetate adhesives (PVAc, JUJU‐8708) and have lower emissions of VOCs. As an environmentally‐friendly adhesive for wood‐based substrates, this adhesive may have potential applications in the wood processing industry. [ABSTRACT FROM AUTHOR]

Using water as a hydrogen/oxygen source for electrocatalytic production of high-value chemicals is highly desirable from a sustainability perspective due to the pivotal role of reduction/oxidation reactions in chemical industry. However, competition from water splitting into H2/O2 typically limits the electron efficiency and process economy. In this work, an oxygen vacancy-rich NiFe-layered double hydroxide (NiFe-LDH)-derived catalyst was obtained by the reduction of monolayer NiFe-LDH (NiFe-mono) at 400 °C in a 10% H2/Ar atmosphere. NiFe-400 showed outstanding activity for the electrocatalytic reduction of p-nitrophenol (p-NP) to p-aminophenol (p-AP) in 1 M KOH, delivering a faradaic efficiency (FE) above 99%. Under continuous electrolytic reduction conditions, 97% FE could be maintained even at 100 mM p-NP. In situ XAFS and DFT theoretical calculations revealed that the Fe site is the main active site, and the existence of oxygen defects promotes the interaction between the active site and the intermediate of the p-NP hydrogenation reaction. Furthermore, in order to utilize the oxygen evolved by water splitting, a paired electrolysis cell was developed that allowed the simultaneous reduction of p-NP to p-AP over NiFe-LDH at the cathode and 5-hydroxymethylfurfural (HMF) oxidation to 2,5-furandicarboxylic acid (FDCA) over a monolayered NiCo-LDH catalyst (NiCo-mono) at the anode, with the combined anode and cathode FE being >190%. Results encourage the wider use of defect-rich LDHs in green chemical synthesis with water as a hydrogen/oxygen source. [ABSTRACT FROM AUTHOR]

Private set union (PSU) allows several parties to obtain the union of their private sets without disclosing each party's private information. Existing PSU protocols often have polynomial complexity for the complete set size or complicated process. In this paper, a quantum multi-party PSU protocol based on least common multiple (LCM) and Shor's algorithm is proposed, which enables the union of multiple sets to be computed all at once. In order to increase the one-time success probability of the protocol, we first improved Shor's period-finding algorithm, which is used in LCM computation and integer factoring. Each party's private set is encoded into an integer obtained by multiplying several prime numbers, thus the PSU problem is transformed into an LCM problem. The LCM of these integers is computed by using the improved Shor's period-finding algorithm, and then factored to derived the union set. We prove the correctness of the proposed protocol, and its unconditional security against semi-honest attacks. Complexity analysis shows that our protocol has logarithmic complexity for the complete set size. [ABSTRACT FROM AUTHOR]

Classical forgery attacks against Offset Two-round (OTR) structures require some harsh conditions, such as some plaintext and ciphertext pairs need to be known, and the success probability is not too high. To solve these problems, a quantum forgery attack on OTR structure using Simon's algorithm is proposed. The attacker intercepts the ciphertext-tag pair (C , T) between the sender and receiver, while Simon's algorithm is used to find the period of the tag generation function in OTR, then we can successfully forge new ciphertext C ′ ( C ′ ≠ C) for intercepted tag T. For a variant of OTR structure (Prøst-OTR-Even-Mansour structure), a universal forgery attack, in which it is easy to generate the correct tag of any given message if the attacker is allowed to change a single block in it, is proposed. It first obtains the secret parameter L using Simon's algorithm, then the secret parameter L is used to find the keys k 1 and k 2 , so that an attacker can forge the changed messages. It only needs several plaintext blocks to help obtain the keys to forge any messages. Performance analysis shows that the query complexity of our attack is O (n) , and its success probability is very close to 1. [ABSTRACT FROM AUTHOR]