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Summary: In this article, we study parameter estimation problems for fractional commensurate Hammerstein systems utilizing the conformable fractional derivative. Two algorithms are investigated: first, the Poisson moment functions (PMF) method, aiming to transfer the fractional derivative of the measurement signal into PMF using the fractional Laplace transform and convolution; second, a proposed new instrumental variable algorithm, which is based on the conformable fractional derivative. Both algorithms have been analyzed and shown to be consistent. A comprehensive complexity analysis is provided for each algorithm. Furthermore, a kind of special time‐varying systems are discussed under the conformable fractional derivative. Finally, an example is given to illustrate the effectiveness of the proposed algorithms. [ABSTRACT FROM AUTHOR]

Type I main‐chain polyrotaxanes (PRs) with multiple wheels threaded onto the axle are widely employed to design slide‐ring materials. However, Type II main‐chain PRs with axles threading into the macrocycles on the polymer backbones have rarely been studied, although they feature special topological structures and dynamic characteristics. Herein, we report the design and preparation of Type II main‐chain PR‐based mechanically interlocked networks (PRMINs), based on which the relationship between microscopic motion of mechanical bonds on the PRs and macroscopic mechanical performance of materials has been revealed. The representative PRMIN‐2 exhibits a robust feature in tensile tests with high stretchability (1680 %) and toughness (47.5 MJ/m3). Moreover, it also has good puncture performance with puncture energy of 22.0 mJ. Detailed rheological measurements and coarse‐grained molecular dynamics (CGMD) simulation reveal that the embedded multiple [2]rotaxane mechanical bonds on the PR backbones of PRMINs could undergo a synergistic long‐range sliding motion under external force, with the introduction of collective dangling chains into the network. As a result, the synchronized motions of coherent PR chains can be readily activated to accommodate network deformation and efficiently dissipate energy, thereby leading to enhanced mechanical performances of PRMINs. [ABSTRACT FROM AUTHOR]

Polyrotaxanes (PRs) have attracted significant research attention due to their unique topological structures and high degrees of conformational freedom. Herein, we take advantage of an oligo[2]rotaxane to construct a novel class of dynamically cross‐linked rotaxane network (DCRN) mediated by metal‐coordination. The oligo[2]rotaxane skeleton offers several distinct advantages: In addition to retaining the merits of traditional polymer backbones, the ordered intramolecular motion of the [2]rotaxane motifs introduced dangling chains into the network, thereby enhancing the stretchability of the DCRN. Additionally, the dissociation of host–guest recognition and subsequent sliding motion, along with the breakage of metal‐coordination interactions, represented an integrated energy dissipation pathway to enhance mechanical properties. Moreover, the resulting DCRN demonstrated responsiveness to multiple stimuli and displayed exceptional self‐healing capabilities in a gel state. Upon exposure to PPh3, which induced network deconstruction by breaking the coordinated cross‐linking points, the oligo[2]rotaxane could be recovered, showcasing good recyclability. These findings demonstrate the untapped potential of the oligo[2]rotaxane as a polymer skeleton to develop DCRN and open the door to extend their advanced applications in intelligent mechanically interlocked materials. [ABSTRACT FROM AUTHOR]

Adhesives have been widely used to splice and repair materials to meet practical needs of humanity for thousands of years. However, developing robust adhesives with balanced adhesive and cohesive properties still remains a challenging task. Herein, we report the design and preparation of a robust mechanically interlocked [an]daisy chain network (DCMIN) adhesive by orthogonal integration of mechanical bonds and 2‐ureido‐4[1H]‐pyrimidone (UPy) H‐bonding in a single system. Specifically, the UPy moiety plays a dual role: it allows the formation of a cross‐linked network and engages in multivalent interactions with the substrate for strong interfacial bonding. The mechanically interlocked [an]daisy chain, serving as the polymeric backbone of the adhesive, is able to effectively alleviate applied stress and uphold network integrity through synergistic intramolecular motions, and thus significantly improves the cohesive performance. Comparative analysis with the control made of the same quadruple H‐bonding network but with non‐interlocked [an]daisy chain backbones demonstrates that our DCMIN possesses superior adhesion properties over a wide temperature range. These findings not only contribute to a deep understanding of the structure‐property relationship between microscopic mechanical bond motions and macroscopic adhesive properties but also provide a valuable guide for optimizing design principles of robust adhesives. [ABSTRACT FROM AUTHOR]

Fire significantly contributes to greenhouse gas emissions. The current global burned area (BA) products mainly have coarse native spatial resolution, which leads to underestimation of global BA and carbon emissions from biomass burning. Performances of BA products in Africa from GABAM (30 m), MCD64A1 (500 m), GFED4s (0.25°), FireCCI51 (250 m), and GFED5 (0.25°) were compared. From 2014 to 2020, GFED5 detected the most BA, 1.58 times more than GABAM during the same period. GABAM detected 0.09 Mkm2 more burned area than FireCCI51 on average. From 2014 to 2016, GABAM detected an average of 2.99 Mkm2 of BA in Africa, which was 1.03 times more than GFED4s. From 2014 to 2021, the average African BA derived from GABAM was 2.89 Mkm2, 1.22 times more than MCD64A1. The increase in BA will inevitably lead to an increase in the estimation of carbon emissions from biomass burning. Based on GABAM products and GFED framework, we estimated the average vegetation burning carbon emissions in Africa from 2014 to 2021 to be 1113.25 Tg, which is higher than GFED4s' carbon emissions in the same time period. This shows that the use of high‐resolution (30 m) burned area products to estimate carbon emissions can effectively avoid the underestimation of overall fire carbon emissions. Plain Language Summary: Biomass burning is a significant contributor to climate change, and Africa is a hotspot for fire activity. Africa accounts for around 70% of the global burned area (BA) and 50% of the global carbon emissions from biomass burning. However, current coarse native spatial resolution burned area products over Africa underestimate the true burning situation in Africa and mask the full impact of African biomass burning on global greenhouse gases and aerosols. To address this issue, we employ novel high spatial resolution (30 m) BA products of Africa from 2014 to 2021, which markedly enhance the identification of burned area and estimation of biomass burning carbon emissions. This study yields novel data and research conclusions that contribute to a better understanding of burned area and fire‐induced carbon emissions in Africa. Key Points: Carbon emissions from biomass combustion in Africa during 2014–2021 are estimated using 30 m BA products30 m BA products enhance small fire detection and boundary delineationAfrica still needs higher spatial and temporal resolution burned area products [ABSTRACT FROM AUTHOR]

The pursuit of fabricating high‐performance graphene films has aroused considerable attention due to their potential for practical applications. However, developing both stretchable and tough graphene films remains a formidable challenge. To address this issue, we herein introduce mechanical bond to comprehensively improve the mechanical properties of graphene films, utilizing [2]rotaxane as the bridging unit. Under external force, the [2]rotaxane cross‐link undergoes intramolecular motion, releasing hidden chain and increasing the interlayer slip distance between graphene nanosheets. Compared with graphene films without [2]rotaxane cross‐linking, the presence of mechanical bond not only boosted the strength of graphene films (247.3 vs 74.8 MPa) but also markedly promoted the tensile strain (23.6 vs 10.2 %) and toughness (23.9 vs 4.0 MJ/m3). Notably, the achieved tensile strain sets a record high and the toughness surpasses most reported results, rendering the graphene films suitable for applications as flexible electrodes. Even when the films were stretched within a 20 % strain and repeatedly bent vertically, the light‐emitting diodes maintained an on‐state with little changes in brightness. Additionally, the film electrodes effectively actuated mechanical joints, enabling uninterrupted grasping movements. Therefore, the study holds promise for expanding the application of graphene films and simultaneously inspiring the development of other high‐performance two‐dimensional films. [ABSTRACT FROM AUTHOR]

An adaptive particle refinement (APR) algorithm has been developed for the smoothed particle hydrodynamics (SPH) method to augment the resolution of the region of interest to achieve high accuracy and simultaneously reduce the cost of computational resources. It is widely applied in the field of fluid-controlling problems involving large interface deformations, such as the two-phase flow and fluid–structure interaction because this algorithm can capture the interface with high accuracy. Nonetheless, existing APR algorithms widely encounter computational dispersion issues at the interface of regions of different particle resolutions. Moreover, traditional shifting algorithms applied in the APR processes also have difficulties in dealing with particles with different smooth lengths. In this work, an algorithm for fast particle generation was first developed based on the accelerated ray method, which accelerates the discretization of the flow field into particles. Then, a dynamic refinement/coarsening algorithm based on the APR algorithm is proposed to solve the computational dispersion problem that occurs at the refinement/coarsening interfaces. In addition, the shifting algorithm was improved in this work to ensure the particles are always well distributed during numerical calculations and, thus, can efficiently facilitate the adaptive particle refinement/coarsening processes. Comparative analysis indicates that the robust algorithms developed for the SPH method in this work can lead to more precise and reasonable flow fields compared with the conventional SPH adaptive methods. [ABSTRACT FROM AUTHOR]

Metal-free graphitic carbon nitride (g-C3N4) has captured significant attention as a low-cost and efficient hydrogen production photocatalyst through. Effectively regulating the microstructure and accelerating the separation of photogenerated carriers remain crucial strategies for promoting the photocatalytic performance of this material. Herein, a novel sulfur–carbon co-doped g-C3N4 (SCCN) hierarchical microtubules filled with abundant nanosheets inside by thermal polymerization is reported. Numerous nanosheets create abundant pores and cavities inside the SCCN microtubes, thereby increasing the specific surface area of g-C3N4 and providing sufficient reactant attachment sites. Besides, the hierarchical structure of SCCN microtubules strengthens the reflection and scattering of light, and the utilization of visible light is favorably affected. More importantly, co-doping S and C has greatly improved the photocatalytic performance of graphitic carbon nitride, optimized the band gap structure and enhanced the photogenerated carrier splitting. Consequently, the SCCN exhibits a remarkable photocatalytic H2 evolution rate of 4868 µmol/(g·h). This work demonstrates the potential of multi-nonmetal doped g-C3N4 as the ideal photocatalyst for H2 evolution. [ABSTRACT FROM AUTHOR]

Covalent polymer networks find wide utility in diverse engineering applications owing to their desirable stiffness and resilience. However, the rigid covalent chemical structure between crosslinking points imposes limitations on enhancing their toughness. Although the incorporation of sacrificial chemical bonds has shown promise in improving toughness through energy dissipation, composite networks struggle to maintain both rapid recovery and stiffness. Consequently, a significant challenge persists in achieving a covalent network that combines high strength, stiffness, toughness, and fast recovery performance. To address this challenge, we propose a novel sacrificial structure termed “sacrificial conformation.” In this approach, β‐cyclodextrin is covalently embedded into the network skeleton as the sacrificial conformation element. Compared to traditional covalent networks (LCN), well‐designed cyclodextrin‐embedded covalent network (CCN) exhibit a 100‐fold increase in Young's modulus and a 60‐fold increase in toughness. Importantly, CCN maintains excellent elasticity, ensuring swift recovery after deformation. This sacrificial conformational strategy enables efficient energy dissipation without necessitating the rupture of chemical bonds, thereby overcoming the limitations of traditional approaches. This advancement holds great promise for the design and fabrication of advanced elastomers and hydrogels with superior mechanical properties and dynamic behavior. [ABSTRACT FROM AUTHOR]

Artificial wrinkles, especially those with responsive erasure/regeneration behaviors have gained extensive interest due to their potential in smart applications. However, current wrinkle modulation methods primarily rely on network rearrangement, causing bottlenecks in in situ wrinkle regeneration. Herein, we report a dually cross-linked network wherein [2]rotaxane cross-link can dissipate stress within the wrinkles through its sliding motion without disrupting the network, and quadruple H-bonding cross-link comparatively highlight the advantages of [2]rotaxane modulation. Acid stimulation dissociates quadruple H-bonding and destructs network, swiftly eliminating the wrinkles. However, the regeneration process necessitates network rearrangement, making in situ recovery unfeasible. By contrast, alkaline stimulation disrupts host-guest recognition, and subsequent intramolecular motion of [2]rotaxane dissipate energy to eliminate wrinkles gradually. The always intact network allows for the in situ recovery of surface microstructures. The responsive behaviors of quadruple H-bonding and mechanical bond are orthogonal, and their combination leads to wrinkles with multiple but accurate responsiveness., (© 2024. The Author(s).)

Loops are prevalent topological structures in cross-linked polymer networks, resulting from the folding of polymer chains back onto themselves. Traditionally, they have been considered as defects that compromise the mechanical properties of the network, leading to extensive efforts in synthesis to prevent their formation. In this study, we introduce the inclusion of cyclic dibenzo-24-crown-8 (DB24C8) moieties within the polymer network strands to form CCNs, and surprisingly, these loops enhance the mechanical performances of the network, leading to tough elastomers. The toughening effect can be attributed to the unique cyclic structure of DB24C8. The relatively small size and the presence of rigid phenyl rings provide the loops with relatively stable conformations, allowing for substantial energy dissipation upon the application of force. Furthermore, the DB24C8 rings possess a broad range of potential conformations, imparting the materials with exceptional elasticity. The synergistic combination of these two features effectively toughens the materials, resulting in a remarkable 66-fold increase in toughness compared to the control sample of covalent networks. Moreover, the mechanical properties, particularly the recovery performance of the network, can be effectively tuned by introducing guests to bind with DB24C8, such as potassium ions and secondary ammonium salts., (© 2024 Wiley‐VCH GmbH.)