Cross-linking Copolymerization of Acrylic Acid and Multi-armed Cross-linkers

The overall cross-linking copolymerization of acrylic acid and multi-armed cross-linkers are investigated by in situ interferometry. The results show that the more arms the cross-linkers have, the higher the polymerization rate is. However, they also mean the existence of less cross-linking efficiency and some defects in gel network.

Starlet:Network defense resource allocation with multi-armed bandits for cloud-edge crowd sensing in IoT

The cloud platform has limited defense resources to fully protect the edge servers used to process crowd sensing data in Internet of Things.To guarantee the network's overall security,we present a network defense resource allocation with multi-armed bandits to maximize the network's overall benefit.Firstly,we propose the method for dynamic setting of node defense resource thresholds to obtain the defender(attacker)benefit function of edge servers(nodes)and distribution.Secondly,we design a defense resource sharing mechanism for neighboring nodes to obtain the defense capability of nodes.Subsequently,we use the decomposability and Lipschitz conti-nuity of the defender's total expected utility to reduce the difference between the utility's discrete and continuous arms and analyze the difference theoretically.Finally,experimental results show that the method maximizes the defender's total expected utility and reduces the difference between the discrete and continuous arms of the utility.

Distributed Weighted Data Aggregation Algorithm in End-to-Edge Communication Networks Based on Multi-armed Bandit

As a combination of edge computing and artificial intelligence,edge intelligence has become a promising technique and provided its users with a series of fast,precise,and customized services.In edge intelligence,when learning agents are deployed on the edge side,the data aggregation from the end side to the designated edge devices is an important research topic.Considering the various importance of end devices,this paper studies the weighted data aggregation problem in a single hop end-to-edge communication network.Firstly,to make sure all the end devices with various weights are fairly treated in data aggregation,a distributed end-to-edge cooperative scheme is proposed.Then,to handle the massive contention on the wireless channel caused by end devices,a multi-armed bandit(MAB)algorithm is designed to help the end devices find their most appropriate update rates.Diffe-rent from the traditional data aggregation works,combining the MAB enables our algorithm a higher efficiency in data aggregation.With a theoretical analysis,we show that the efficiency of our algorithm is asymptotically optimal.Comparative experiments with previous works are also conducted to show the strength of our algorithm.

Mechanism of high Li-ion conductivity in poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network based electrolyte revealed by solid-state NMR

Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid electrolytes.Cross-linked polymers have the potential to further improve the mechanical property without trading off Li-ion conductivity.In this study,focusing on a recently developed cross-linked SPE,i.e.,the one based on poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network(PVCN),we used solid-state nuclear magnetic resonance(NMR)techniques to investigate the fundamental interaction between the chain segments and Li ions,as well as the lithium-ion motion.By utilizing homonuclear/heteronuclear correlation,CP(cross-polarization)kinetics,and spin-lattice relaxation experiments,etc.,we revealed the structural characteristics and their relations to lithium-ion mobilities.It is found that the network formation prevents poly(ethylene oxide)chains from crystallization,which could create sufficient space for segmental tumbling and Li-ion co nductio n.As such,the mechanical property is greatly improved with even higher Li-ion mobilities compared to the poly(vinylene carbonate)or poly(ethylene oxide)based SPE analogues.

Residual alkali-evoked cross-linked polymer layer for anti-air-sensitivity LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)cathode

High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)faces challenges related to capacity decay caused by residual alkalis owing to high sensitivity to air.To address this issue,we propose a hazardous substances upcycling method that fundamentally mitigates alkali content and concurrently induces the emergence of an anti-air-sensitive layer on the cathode surface.Through the neutralization of polyacrylic acid(PAA)with residual alkalis and then coupling it with 3-aminopropyl triethoxysilane(KH550),a stable and ion-conductive cross-linked polymer layer is in situ integrated into the LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)(NCM)cathode.Our characterization and measurements demonstrate its effectiveness.The NCM material exhibits impressive cycling performance,retaining 88.4%of its capacity after 200 cycles at 5 C and achieving an extraordinary specific capacity of 170.0 mA h g^(-1) at 10 C.Importantly,this layer on the NCM efficiently suppresses unfavorable phase transitions,severe electrolyte degradation,and CO_(2)gas evolution,while maintaining commendable resistance to air exposure.This surface modification strategy shows widespread potential for creating air-stable LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)cathodes,thereby advancing high-performance LIBs.

Tuning the cross-linked structure of basic poly(ionic liquid)to develop an efficient catalyst for the conversion of vinyl carbonate to dimethyl carbonate

Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium methoxide basic catalyst to produce DMC through the transesterification reaction between vinyl carbonate and methanol.However,the utilization of this catalyst presents several challenges during the process,including equipment corrosion,the generation of solid waste,susceptibility to deactivation,and complexities in separation and recovery.To address these limitations,a series of alkaline poly(ionic liquid)s,i.e.[DVBPIL][PHO],[DVCPIL][PHO],and[TBVPIL][PHO],with different crosslinking degrees and structures,were synthesized through the construction of cross-linked polymeric monomers and functionalization.These poly(ionic liquid)s exhibit cross-linked structures and controllable cationic and anionic characteristics.Research was conducted to investigate the effect of the cross-linking degree and structure on the catalytic performance of transesterification in synthesizing DMC.It was discovered that the appropriate cross-linking degree and structure of the[DVCPIL][PHO]catalyst resulted in a DMC yield of up to 80.6%.Furthermore,this catalyst material exhibited good stability,maintaining its catalytic activity after repeated use five times without significant changes.The results of this study demonstrate the potential for using alkaline poly(ionic liquid)s as a highly efficient and sustainable alternative to traditional catalysts for the transesterification synthesis of DMC.

Early changes in corneal densitometry after FS-LASIK combined with accelerated corneal cross-linking for correction of high myopia

AIM:To observe the effects of femtosecond laserassisted excimer laser in situ keratomileusis combined with accelerated corneal cross-linking(FS-LASIK Xtra)on corneal densitometry after correcting for high myopia.METHODS:In this prospectively study,130 patients underwent FS-LASIK or FS-LASIK Xtra for high myopia.Their right eyes were selected for inclusion in the study,of which 65 cases of 65 eyes in the FS-LASIK group,65 patients with 65 eyes in the FS-LASIK Xtra group.Patients were evaluated for corneal densitometry at 1,3,and 6mo postoperatively using Pentacam Scheimpflug imaging.RESULTS:Preoperative differences in corneal densitometry between the FS-LASIK and FS-LASIK Xtra groups in different ranges were not statistically significant(P>0.05).Layer-by-layer analysis revealed statistically significant differences in the anterior(120μm),central,and total layer corneal densitometry between the FS-LASIK and FS-LASIK Xtra groups at 1 and 3mo postoperatively(all P<0.05),the FS-LASIK Xtra group is higher than that of the FS-LASIK group.Analysis of different diameter ranges showed statistically significant differences between the FS-LASIK group and the FS-LASIK Xtra group at 1mo postoperatively in the ranges of 0–2,2–6,and 6–10 mm(both P<0.05);At 3mo postoperatively,the FS-LASIK Xtra group is higher than that of the FS-LASIK group in the ranges of 0–2 and 2–6 mm(P<0.05).At 6mo postoperatively,there were no statistically significant differences in corneal densitometry between the FS-LASIK group and the FS-LASIK Xtra group in different diameter ranges(all P>0.05).CONCLUSION:There is an increase in internal corneal densitometry during the early postoperative period after FS-LASIK Xtra for correction of high myopia.However,the densitometry values decreased to the level of conventional FS-LASIK at 6mo after surgery,with the most significant changes observed in the superficial central zone.

Assisted Compatibility, and Balanced Regulation of the Mechanical, Thermal, and Antioxidant Activity of Polyvinyl Alcohol-Chinese Bayberry Tannin Extract Films Using Different Di-Aldehydes as Cross-Linkers

Polyvinyl alcohol(PVA)-based films containing Chinese bayberry tannin(BT)were prepared by cross-linking using glyoxal,glutaraldehyde and dialdehyde starch,individually.The presence of cross-linkers was evident to promote the transparency and decrease the moisture content of PVA/BT films,while the water solubility stayed almost unchanged in the cross-linked PVA/BTfilms.All cross-linkers provided promotion of the water vapor per-meability,mechanical property and thermal stability of PVA/BT films.The best water vapor barrier capacity was found in case of glutaraldehyde cross-linked PVA/BT film,while the highest tensile strength was encountered in case of glyoxal cross-linked PVA/BT films,compared with the uncross-linked films.The scavenging action of the films towards DPPH radical activity was influenced by the nature of each cross-linker.Namely,the PVA/AT film cross-linked by glutaraldehyde acquired the lowest radical scavenging activity in a certain time,suggesting that glutaraldehyde decreased the release rate of BT from PVA.Based on the experimental data,glutaraldehyde and dialdehyde starch could be more suitable for PVA/BT film preparation since they can promote the intermo-lecular interaction of PVA and BT to a reasonable extent.

Construction of all-organic low dielectric polyimide hybrids via synergistic effect between covalent organic framework and cross-linking structure

Polyimide(PI)is a promising electronic packaging material,but it remains challenging to obtain an all-organic PI hybrid film with decreased dielectric constant and loss without modifying the monomer.Herein,a series of allorganic PI hybrid films were successfully prepared by introducing the covalent organic framework(COF),which could induce the formation of the cross-linking structure in the PI matrix.Due to the synergistic effects of the COF fillers and the cross-linking structure,the PI/COF hybrid film containing 2 wt%COF exhibited the lowest dielectric constant of 2.72 and the lowest dielectric loss(tanδ)of 0.0077 at 1 MHz.It is attributed to the intrinsic low dielectric constant of COF and a large number of mesopores within the PI.Besides,the cross-linking network of PI prevents the molecular chains from stacking and improves the fraction of free volume(FFV).The molecular dynamics simulation results are well consistent with the dielectric properties data.Furthermore,the PI/COF hybrid film with 5 wt%COF showed a significant enhancement in breakdown strength,which increased to 412.8 kV/mm as compared with pure PI.In addition,the PI/COF hybrid film achieve to reduce the dielectric constant and thermal expansion coefficient(CTE).It also exhibited excellent thermal,hydrophobicity,and mechanical performance.The all-organic PI/COF hybrid films have great commercial potential as next-generation electronic packaging materials.

In situ formed cross-linked polymer networks as dual-functional layers for high-stable lithium metal batteries

Lithium-metal anodes(LMAs)have been recognized as the ultimate anodes for next-generation batteries with high energy density,but stringent assembly-environment conditions derived from the poor moisture stability dramatically hinder the transformation of LMAs from laboratory to industry.Herein,an in situ formed cross-linked polymer layer on LMAs is designed and constructed by a facile thiol-acrylate click chemistry reaction between poly(ethylene glycol)diacrylate(PEGDA)and the crosslinker containing multi thiol groups under UV irradiation.Owing to the hydrophobic nature of the layer,the treated LMAs demonstrate remarkable humid stability for more than 3 h in ambient air(70%relative humidity).The coating humid-resistant protective layer also possesses a dual-functional characterization as solid polymer electrolytes by introducing lithium bis(trifluoromethanesulfonyl)imide in the system in advance.The intimate contact between the polymer layer and LMAs reduces interfacial resistance in the assembled Li/LiFePO_(4)or Li/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)full cell effectively,and endows the cell with an outstanding cycle performance.

Mechanical Properties of Silicone Rubber Using Carbosilane Dendrimers as the Cross-linker

Peroxide-cured high-temperature vulcanized （HTV） silicone rubber was prepared by using allyl-capped carbosilane dendrimers, in which the core molecule is Si（CHaCH=CH2）4, as the cross-linker. It showed that this kind of allyl-capped carbosilane dendrimer improved the mechanical properties of silicone rubber.

Small molecule interfacial cross-linker for highly efficient two-dimensional perovskite solar cells

The nonradiative recombination of charge carriers at the hole transport layer(HTL)/perovskite interface generally induces remarkable performance loss of the inverted two-dimensional perovskite solar cells(2D PSCs). Herein, a cross-linkable small molecule of 2-mercaptoimidazole(2-MI) was introduced into the nickel oxide(NiO_(x))/2D perovskite interface. Experiments have confirmed the formation of Ni-N covalent bond by N atom in the 2-MI and Ni in the NiO_(x) and the coordinating between S atom of 2-MI and under-coordinated Pb^(2+) near to the NiO_(x)/perovskite interface, which contributes to creating a crosslinking between NiO_(x)/perovskite interface to restrain charge carrier recombination and enhance the extraction of hole carriers at the interface. Besides, the 2-MI modification layer is also beneficial for promoting the crystallinity of 2D perovskite. Consequently, the inverted 2D PSCs with 2-MI modification achieved the best power conversion efficiency of 15%. This paves a route to acquire highly efficient 2D PSCs by constructing a cross-linking at the NiO_(x)HTL/2D perovskite interface.

Strict greedy design paradigm applied to the stochastic multi-armed bandit problem

The process of making decisions is something humans do inherently and routinely,to the extent that it appears commonplace. However,in order to achieve good overall performance,decisions must take into account both the outcomes of past decisions and opportunities of future ones. Reinforcement learning,which is fundamental to sequential decision-making,consists of the following components: 1 A set of decisions epochs; 2 A set of environment states; 3 A set of available actions to transition states; 4 State-action dependent immediate rewards for each action.At each decision,the environment state provides the decision maker with a set of available actions from which to choose. As a result of selecting a particular action in the state,the environment generates an immediate reward for the decision maker and shifts to a different state and decision. The ultimate goal for the decision maker is to maximize the total reward after a sequence of time steps.This paper will focus on an archetypal example of reinforcement learning,the stochastic multi-armed bandit problem. After introducing the dilemma,I will briefly cover the most common methods used to solve it,namely the UCB and εn- greedy algorithms. I will also introduce my own greedy implementation,the strict-greedy algorithm,which more tightly follows the greedy pattern in algorithm design,and show that it runs comparably to the two accepted algorithms.

Training a Quantum Neural Network to Solve the Contextual Multi-Armed Bandit Problem

Artificial intelligence has permeated all aspects of our lives today. However, to make AI behave like real AI, the critical bottleneck lies in the speed of computing. Quantum computers employ the peculiar and unique properties of quantum states such as superposition, entanglement, and interference to process information in ways that classical computers cannot. As a new paradigm of computation, quantum computers are capable of performing tasks intractable for classical processors, thus providing a quantum leap in AI research and making the development of real AI a possibility. In this regard, quantum machine learning not only enhances the classical machine learning approach but more importantly it provides an avenue to explore new machine learning models that have no classical counterparts. The qubit-based quantum computers cannot naturally represent the continuous variables commonly used in machine learning, since the measurement outputs of qubit-based circuits are generally discrete. Therefore, a continuous-variable (CV) quantum architecture based on a photonic quantum computing model is selected for our study. In this work, we employ machine learning and optimization to create photonic quantum circuits that can solve the contextual multi-armed bandit problem, a problem in the domain of reinforcement learning, which demonstrates that quantum reinforcement learning algorithms can be learned by a quantum device.

Synthesis and Properties of Polyurethane Elastomers Containing Sucrose as a Cross-Linker

Polyaddition using isocyanate and polyol forms polyurethane elastomer (PUE). However, this method has rarely been applied to the construction of PUEs containing sucrose. Hence, the introduction of sucrose (disaccharide) as a cross-linker via polyaddition remains a challenging subject in polymer chemistry. Here, we report the synthesis of PUEs using an aromatic isocyanate (4,4’-diphenylmethane diisocyanate), polyols including a polyether polyol (polytetramethylene glycol) and two polyester polyols (polycaprolactone and polycarbonate diols), and sucrose as a crosslinker by a one-shot method. The PUEs containing sucrose were successfully produced. The use of sucrose was essential to obtain the desired PUEs containing sucrose units in the main chain.

Stochastic programming based multi-arm bandit offloading strategy for internet of things

In order to solve the high latency of traditional cloud computing and the processing capacity limitation of Internet of Things(IoT)users,Multi-access Edge Computing(MEC)migrates computing and storage capabilities from the remote data center to the edge of network,providing users with computation services quickly and directly.In this paper,we investigate the impact of the randomness caused by the movement of the IoT user on decision-making for offloading,where the connection between the IoT user and the MEC servers is uncertain.This uncertainty would be the main obstacle to assign the task accurately.Consequently,if the assigned task cannot match well with the real connection time,a migration(connection time is not enough to process)would be caused.In order to address the impact of this uncertainty,we formulate the offloading decision as an optimization problem considering the transmission,computation and migration.With the help of Stochastic Programming(SP),we use the posteriori recourse to compensate for inaccurate predictions.Meanwhile,in heterogeneous networks,considering multiple candidate MEC servers could be selected simultaneously due to overlapping,we also introduce the Multi-Arm Bandit(MAB)theory for MEC selection.The extensive simulations validate the improvement and effectiveness of the proposed SP-based Multi-arm bandit Method(SMM)for offloading in terms of reward,cost,energy consumption and delay.The results showthat SMMcan achieve about 20%improvement compared with the traditional offloading method that does not consider the randomness,and it also outperforms the existing SP/MAB based method for offloading.

Cross-Linking of Sago Starch with Furan and Bismaleimide via the Diels-Alder Reaction

This research paper describes the synthesis of thermo-reversible cross-linking of sago starch by grafting a furan pendant group(methyl 2-furoate)onto the starch backbone,followed by a Diels-Alder(DA)reaction of the furan functional group with 1,1′-(methylenedi-4,1-phenylene)bismaleimide(BM).The proof of principles was provided by FTIR and 1H-NMR analyses.The relevant FTIR peaks are the carbonyl peak(υC=O sym)at 1721 cm^(−1);the two peaks appeared after DA cross-linking,i.e.,at 1510 cm^(−1)(corresponding toυCH=CH BM aromatic rings,stretching vibrations),and at 1173 cm^(−1)(assigned to cycloadduct(C-O-C,δDA ring))while the^(1)H-NMR result shows evidence for the presence of a furan ring in the starch matrices(in the range ofδ6.3-7.5 ppm).The crosslinked starch product is indeed thermally reversible,as is evident from the appearance of exothermal(DA,temperature range of 50℃-70℃)and endothermal(retro DA,temperature range of 125℃-150℃)transitions in the DSC thermograms.This paper not only proves the thermal reversibility but also demonstrates that the final product properties(chemical,morphology,and thermal stability)can be tuned by varying the annealing temperature,BM intake,and reaction time.

Cross-linked polyelectrolyte reinforced SnO_(2)electron transport layer for robust flexible perovskite solar cells

SnO_(2)electron transport layer(ETL)is a vital component in perovskite solar cells(PSCs),due to its excellent photoelectric properties and facile fabrication process.In this study,we synthesized a water-soluble and adhesive polyelectrolyte with ethanolamine(EA)and poly-acrylic acid(PAA).The linear PAA was crosslinked by EA,forming a 3D network that stabilized the SnO_(2)nanoparticle dispersion.An organic–inorganic hybrid ETL is developed by introducing the cross-linked PAA-EA into SnO_(2)ETL,which prevents nano particle agglomeration and facilitates uniform SnO_(2)film formation with fewer defects.Additionally,the PAA-EA-modified SnO_(2)facilitated a uniform and compact perovskite film,enhancing the interface contact and carrier transport.Consequently,the PAA-EA-modified PSCs exhibited excellent PCE of 24.34%and 22.88%with high reproducibility for areas of 0.045 and 1.00 cm~2,respectively.Notably,owing to structure reinforce effect of PAA-EA in SnO_(2)ETL,flexible device demonstrated an impressive PCE of 23.34%while maintaining 90.1%of the initial PCE after 10,000 bending cycles with a bending radius of 5 mm.This successful approach of polyelectrolyte reinforced hybrid organic–inorganic ETL displays great potential for flexible,large-area PSCs application.

A Self-Healing and Nonflammable Cross-Linked Network Polymer Electrolyte with the Combination of Hydrogen Bonds and Dynamic Disulfide Bonds for Lithium Metal Batteries

The self-healing solid polymer electrolytes(SHSPEs)can spontaneously eliminate mechanical damages or micro-cracks generated during the assembly or operation of lithium-ion batteries(LIBs),significantly improving cycling performance and extending service life of LIBs.Here,we report a novel cross-linked network SHSPE(PDDP)containing hydrogen bonds and dynamic disulfide bonds with excellent self-healing properties and nonflammability.The combination of hydrogen bonding between urea groups and the metathesis reaction of dynamic disulfide bonds endows PDDP with rapid self-healing capacity at 28°C without external stimulation.Furthermore,the addition of 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide(EMIMTFSI)improves the ionic conductivity(1.13×10^(−4)S cm^(−1)at 28°C)and non-flammability of PDDP.The assembled Li/PDDP/LiFePO_(4)cell exhibits excellent cycling performance with a discharge capacity of 137 mA h g^(−1)after 300 cycles at 0.2 C.More importantly,the self-healed PDDP can recover almost the same ionic conductivity and cycling performance as the original PDDP.

A UV cross-linked gel polymer electrolyte enabling high-rate and high voltage window for quasi-solid-state supercapacitors

Serving as a promising alternative to liquid electrolyte in the application of portable and wearable devices,gel polymer electrolytes(GPEs)are expected to obtain more preferable properties rather than just be satisfied with the merits of high safety and deformability.Here,an easy-operated method is employed to fabricate cross-linked composite polymer membranes used for GPEs assisted by UV irradiation,in which N-doped carbon quantum dots(N-CQDs)and TiO2are introduced as photocatalysts and additives to improve the performances of GPEs.Specifically,N-CQDs participate as a cross-linker to construct the inner porous structure,and TiO2nanoparticles serve as a stabilizer to improve the electrochemical stability of GPEs under high voltage(3.5 V).The excellent thermal and mechanical stability of the membrane fabricated in this work guarantee the safety of the supercapacitors(SCs).This GPE based SC not only exhibits prominent rate performance(105%capacitance retention at the current density of 40A g^(-1))and cyclic stability(85%at 1 A g^(-1)under 3.5 V after 20,000 cycles),but also displays remarkable energy density(42.88 Wh kg^(-1))with high power density(19.3 k W kg^(-1)).Moreover,the superior rate and cycling performances of the as-prepared GPE based flexible SCs under flat and bending state confirm the feasibility of its application in flexible energy storage devices.