Harness High-Temperature Thermal Energy via Elastic Thermoelectric Aerogels

Despite notable progress in thermoelectric(TE)materials and devices,developing TE aerogels with high-temperature resistance,superior TE performance and excellent elasticity to enable self-powered high-temperature monitoring/warning in industrial and wearable applications remains a great challenge.Herein,a highly elastic,flame-retardant and high-temperature-resistant TE aerogel,made of poly(3,4-ethylene dioxythiophene):poly(styrenesulfonate)/single-walled carbon nanotube(PEDOT:PSS/SWCNT)composites,has been fabricated,displaying attractive compression-induced power factor enhancement.The as-fabricated sensors with the aerogel can achieve accurately pressure stimuli detection and wide temperature range monitoring.Subsequently,a flexible TE generator is assembled,consisting of 25 aerogels connected in series,capable of delivering a maximum output power of 400μW when subjected to a temperature difference of 300 K.This demonstrates its outstanding high-temperature heat harvesting capability and promising application prospects for real-time temperature monitoring on industrial high-temperature pipelines.Moreover,the designed self-powered wearable sensing glove can realize precise wide-range temperature detection,high-temperature warning and accurate recognition of human hand gestures.The aerogel-based intelligent wearable sensing system developed for firefighters demonstrates the desired self-powered and highly sensitive high-temperature fire warning capability.Benefitting from these desirable properties,the elastic and high-temperature-resistant aerogels present various promising applications including self-powered high-temperature monitoring,industrial overheat warning,waste heat energy recycling and even wearable healthcare.

Enhanced High-Temperature Energy Storage Performance of All-Organic Composite Dielectric via Constructing Fiber-Re in forced Structure

Optimizing the high-temperature energy storage characteristics of energy storage dielectrics is of great significance for the development of pulsed power devices and power control systems.Selecting a polymer with a higher glass transition temperature(T_(g))as the matrix is one of the effective ways to increase the upper limit of the polymer operating temperature.However,current high-T_(g)polymers have limitations,and it is difficult to meet the demand for high-temperature energy storage dielectrics with only one polymer.For example,polyetherimide has high-energy storage efficiency,but low breakdown strength at high temperatures.Polyimide has high corona resistance,but low high-temperature energy storage efficiency.In this work,combining the advantages of two polymer,a novel high-T_(g)polymer fiber-reinforced microstructure is designed.Polyimide is designed as extremely fine fibers distributed in the composite dielectric,which will facilitate the reduction of high-temperature conductivity loss for polyimide.At the same time,due to the high-temperature resistance and corona resistance of polyimide,the high-temperature breakdown strength of the composite dielectric is enhanced.After the polyimide content with the best high-temperature energy storage characteristics is determined,molecular semiconductors(ITIC)are blended into the polyimide fibers to further improve the high-temperature efficiency.Ultimately,excellent high-temperature energy storage properties are obtained.The 0.25 vol%ITIC-polyimide/polyetherimide composite exhibits high-energy density and high discharge efficiency at 150℃(2.9 J cm^(-3),90%)and 180℃(2.16 J cm^(-3),90%).This work provides a scalable design idea for high-performance all-organic high-temperature energy storage dielectrics.

TiN/Fe_(2)N/C composite with stable and broadband high-temperature microwave absorption

Facing the complex variable high-temperature environment,electromagnetic wave(EMW)absorbing materials maintaining high stability and satisfying absorbing properties is essential.This study focused on the synthesis and EMW absorbing performance evaluation of TiN/Fe_(2)N/C composite materials,which were prepared using electrostatic spinning followed by a high-temperature nitridation process.The TiN/Fe_(2)N/C fibers constructed a well-developed conductive network that generates considerable conduction loss.The heterogeneous interfaces between different components generated a significant level of interfacial polarization.Thanks to the synergistic effect of stable dielectric loss and optimized impedance matching,the TiN/Fe_(2)N/C composite materials demonstrated excellent and stable absorption performance across a wide temperature range(293-453 K).Moreover,TiN/Fe_(2)N/C-15 achieved a minimum reflection loss(RL)of−48.01 dB and an effective absorption bandwidth(EAB)of 3.64 GHz at 2.1 mm and 373 K.This work provides new insights into the development of high-efficiency and stabile EMW absorbing materials under complex variable high-temperature conditions.

HZSM-5 zeolites undergoing the high-temperature process for boosting the bimolecular reaction in n-heptane catalytic cracking

High-temperature treatment is key to the preparation of zeolite catalysts.Herein,the effects of hightemperature treatment on the property and performance of HZSM-5 zeolites were studied in this work.X-Ray diffraction,N2physisorption,27Al magic angle spinning nuclear magnetic resonance(MAS NMR),and temperature-programmed desorption of ammonia results indicated that the hightemperature treatment at 650℃ hardly affected the inherent crystal and texture of HZSM-5zeolites but facilitated the conversion of framework Al to extra-framework Al,reducing the acid site and enhancing the acid strength.Moreover,the high-temperature treatment improved the performance of HZSM-5 zeolites in n-heptane catalytic cracking,promoting the conversion and light olefins yield while inhibiting coke formation.Based on the kinetic and mechanism analysis,the improvement of HZSM-5 performance caused by high-temperature treatment has been attributed to the formation of extra-framework Al,which enhanced the acid strength,facilitated the bimolecular reaction,and promoted the entropy change to overcome a higher energy barrier in n-heptane catalytic cracking.

Synergistic effect of Zr and Mo on precipitation and high-temperature properties of Al-Si-Cu-Mg alloys

This study focuses on finding a solution to the sharp decline in mechanical properties of Al-Si-Cu-Mg alloys due to rapid coarsening of traditional intermediate phases at high temperature.A new type of modified al oy,to be used in automobile engines at high temperatures,was prepared by adding Zr and Mo into Al-Si-Cu-Mg alloy.The synergistic effects of Zr and Mo on the microstructure evolution and high-temperature mechanical properties were studied.Results show that the addition of Zr and Mo generates a series of intermetallic phases dispersed in the alloy.They can improve the strength of the alloy by hindering dislocation movement and crack propagation.In addition,some nano-strengthened phases show coherent interfaces with the matrix and improve grain refinement.The addition of Mo greatly improves the heat resistance of the alloy.The extremely low diffusivity of Mo enables it to improve the thermal stability of the intermetallic phases,inhibit precipitation during aging,reduce the size of the precipitates,and improve the heat resistance of the alloy.

A review of in-situ high-temperature characterizations for understanding the processes in metallurgical engineering

For the rational manipulation of the production quality of high-temperature metallurgical engineering,there are many challenges in understanding the processes involved because of the black box chemical/electrochemical reactors.To overcome this issue,various in-situ characterization methods have been recently developed to analyze the interactions between the composition,microstructure,and solid-liquid interface of high-temperature electrochemical electrodes and molten salts.In this review,recent progress of in-situ hightemperature characterization techniques is discussed to summarize the advances in understanding the processes in metallurgical engineering.In-situ high-temperature technologies and analytical methods mainly include synchrotron X-ray diffraction(s-XRD),laser scanning confocal microscopy,and X-ray computed microtomography(X-rayμ-CT),which are important platforms for analyzing the structure and morphology of the electrodes to reveal the complexity and variability of their interfaces.In addition,laser-induced breakdown spectroscopy,high-temperature Raman spectroscopy,and ultraviolet-visible absorption spectroscopy provide microscale characterizations of the composition and structure of molten salts.More importantly,the combination of X-rayμ-CT and s-XRD techniques enables the investigation of the chemical reaction mechanisms at the two-phase interface.Therefore,these in-situ methods are essential for analyzing the chemical/electrochemical kinetics of high-temperature reaction processes and establishing the theoretical principles for the efficient and stable operation of chemical/electrochemical metallurgical processes.

Natural Lignin:A Sustainable and Cost-Effective Electrode Material for High-Temperature Na-Ion Battery

Rechargeable sodium-ion batteries usually suffer from accelerated electrode destruction at high temperatures and high synthesis costs of electrode materials.Therefore,it is highly desirable to explore novel organic electrodes considering their cost-effectiveness and large adaptability to volume changes.Herein,natural biomass,pristine lignin,is employed as the sodium-ion battery anodes,and their sodium storage performance is investigated at room temperature and 60℃.The lignin anodes exhibit excellent high-temperature sodium-ion battery performance.This mainly results from the generation of abundant reactive sites(C=O)due to the high temperature-induced homogeneous cleavage of the C_(β)-O bond in the lignin macromolecule.This work can inspire researchers to explore other natural organic materials for large-scale applications and high-value utilization in advanced energy storage devices.

Relationship between hydrogenation degree and pyrolysis performance of jet fuel

Understanding the relationship between the chemical composition and pyrolysis performance of endothermic hydrocarbon fuel(EHF) is of great significance for the design and optimization of advanced EHFs. In this work, the effect of deep hydrogenation on the pyrolysis of commercial RP-3 is investigated.Fuels with different hydrogenation degrees were obtained by the partially and completely catalytic hydrogenation and their pyrolysis performances were investigated using an apparatus equipped with an electrically heated tubular reactor. The results show that with the increase of hydrogenation degree, fuel conversion almost remains constant during the pyrolysis process(500-650°C, 4 MPa);however, the heat sink increases slightly, and the anti-coking performance significantly improves, which are highly related to their H/C ratios. Detailed characterisations reveal that the difference of the pyrolysis performance can be ascribed to the content of aromatics and cycloalkanes: the former are prone to initiate secondary reactions to form coking precursors, while the latter could act as the hydrogen donor and release hydrogen, which will terminate the radical propagation reactions and suppress the coke deposition. This work should provide the guidance for upgrading EHFs by modulating the composition of EHFs.

Understanding the dehydrogenation properties of Mg(0001)/MgH_(2)(110)interface from first principles

Magnesium hydride is one of the most promising solid-state hydrogen storage materials for on-board application.Hydrogen desorption from MgH_(2) is accompanied by the formation of the Mg/MgH_(2) interfaces,which may play a key role in the further dehydrogenation process.In this work,first-principles calculations have been used to understand the dehydrogenation properties of the Mg(0001)/MgH_(2)(110) interface.It is found that the Mg(0001)/MgH_(2)(110) interface can weaken the Mg-H bond.The removal energies for hydrogen atoms in the interface zone are significantly lower compared to those of bulk MgH_(2).In terms of H mobility,hydrogen diffusion within the interface as well as into the Mg matrix is considered.The calculated energy barriers reveal that the migration of hydrogen atoms in the interface zone is easier than that in the bulk MgH_(2).Based on the hydrogen removal energies and diffusion barriers,we conclude that the formation of the Mg(0001)/MgH_(2)(110) interface facilitates the dehydrogenation process of magnesium hydride.

Hybrid 2D/3D Graphitic Carbon Nitride-Based High-Temperature Position-Sensitive Detector

Ultraviolet position-sensitive detectors(PSDs)are expected to undergo harsh environments,such as high temperatures,for a wide variety of applications in military,civilian,and aerospace.However,no report on relevant PSDs operating at high temperatures can be found up to now.Herein,we design a new 2D/3D graphitic carbon nitride(g-C_(3)N_(4))/gallium nitride(GaN)hybrid heterojunction to construct the ultraviolet high-temperature-resistant PSD.The g-C_(3)N_(4)/GaN PSD exhibits a high position sensitivity of 355 mV mm^(-1),a rise/fall response time of 1.7/2.3 ms,and a nonlinearity of 0.5%at room temperature.The ultralow formation energy of-0.917 eV atom^(-1)has been obtained via the thermodynamic phase stability calculations,which endows g-C_(3)N_(4)with robust stability against heat.By merits of the strong built-in electric field of the 2D/3D hybrid heterojunction and robust thermo-stability of g-C_(3)N_(4),the g-C_(3)N_(4)/GaN PSD delivers an excellent position sensitivity and angle detection nonlinearity of 315 mV mm^(-1)and 1.4%,respectively,with high repeatability at a high temperature up to 700 K,outperforming most of the other counterparts and even commercial silicon-based devices.This work unveils the high-temperature PSD,and pioneers a new path to constructing g-C_(3)N_(4)-based harsh-environment-tolerant optoelectronic devices.

Enhanced Ethylene Production from Electrocatalytic Acetylene Semi-hydrogenation Over Porous Carbon-Supported Cu Nanoparticles

Electrocatalytic semi-hydrogenation of acetylene(C_(2)H_(2))over copper nanoparticles(Cu NPs)offers a promising non-petroleum alternative for the green production of ethylene(C2H4).However,server hydrogen evolution reaction(HER)competition in this process prominently decreases C2H4 selectivity,thereby hindering its practical application.Herein,a Cu-based composite catalyst,wherein porous carbon with nanoscale pores was used as a support,is constructed to gather the C_(2)H_(2) feedstocks for suppressing the undesirable HER.As a result,the as-prepared catalyst exhibited C_(2)H_(2) conversion of 27.1%and C_(2)H_(4) selectivity of 88.4%at a C2H4 partial current density of 0.25 A/cm^(2) under optimal−1.0 V versus reversible hydrogen electrode(RHE)under the simulated coal-derived C_(2)H_(2) atmosphere,significantly outperforming the single Cu NPs counterparts.In addition,a series of in situ and ex situ experimental results show that not only the porous nature of the carbon support but also the stabilized Cu^(0)–Cu^(+) dual active sites through the strong metal–support interactions enhance the adsorption capacity of C_(2)H_(2),leading to high C_(2)H_(2) partial pressure,restraining the HER and thus improving the C2H4 selectivity.

Facile molybdenum and aluminum recovery from spent hydrogenation catalyst

Industrial catalyst waste has emerged as a hazardous pollutant that requires safe and proper disposal after the unloading process.Finding a valuable and sustainable strategy for its treatment is a significant challenge compared to traditional methods.In this study,we present a facile method for the recovery of molybdenum and aluminum contents from spent Mo-Ni/Al_(2)O_(3) hydrogenation catalysts through crystallization separation and coprecipitation.Furthermore,the recovered molybdenum and aluminum are utilized as active metals and carriers for the preparation of new catalysts.Their properties were thoroughly analyzed and investigated using various characterization techniques.The hydrogenation activity of these newly prepared catalysts was evaluated on a fixed-bed small-scale device and compared with a reference catalyst synthesized from commercial raw reagents.Finally,the hydrogenation activity of the catalysts was further assessed by using the entire distillate oil of coal liquefaction as the raw oil,specifically focusing on denitrogenation and aromatic saturation.This work not only offers an effective solution for recycling catalysts but also promotes sustainable development.

A Novel Fracturing Fluid with High-Temperature Resistance for Ultra-Deep Reservoirs

Ultra-deep reservoirs play an important role at present in fossil energy exploitation.Due to the related high temperature,high pressure,and high formation fracture pressure,however,methods for oil well stimulation do not produce satisfactory results when conventional fracturing fluids with a low pumping rate are used.In response to the above problem,a fracturing fluid with a density of 1.2~1.4 g/cm^(3)was developed by using Potassium formatted,hydroxypropyl guanidine gum and zirconium crosslinking agents.The fracturing fluid was tested and its ability to maintain a viscosity of 100 mPa.s over more than 60 min was verified under a shear rate of 1701/s and at a temperature of 175℃.This fluid has good sand-carrying performances,a low viscosity after breaking the rubber,and the residue content is less than 200 mg/L.Compared with ordinary reconstruction fluid,it can increase the density by 30%~40%and reduce the wellhead pressure of 8000 m level reconstruction wells.Moreover,the new fracturing fluid can significantly mitigate safety risks.

Microenvironment and electronic state modulation of Pd nanoparticles within MOFs for enhancing low-temperature activity towards DCPD hydrogenation

Precise control of the local environment and electronic state of the guest is an important method of controlling catalytic activity and reaction pathways.In this paper,guest Pd NPs were introduced into a series of host UiO-67 MOFs with different functional ligands and metal nodes,the microenvironment and local electronic structure of Pd is modulated by introducing bipyridine groups and changing metal nodes(Ce_(6)O_(6) or Zr_(6)O_(6)).The bipyridine groups not only promoted the dispersion Pd NPs,but also facilitated electron transfer between Pd and UiO-67 MOFs through the formation of Pd-N bridges.Compared with Zr6 clusters,the tunability and orbital hybridisation of the 4f electronic structure in the Ce_(6) clusters modulate the electronic structure of Pd through the construction of the Ce-O-Pd interfaces.The optimal catalyst Pd/UiO-67(Ce)-bpy presented excellent low-temperature activity towards dicyclopentadiene hydrogenation with a conversion of>99% and a selectivity of>99%(50℃,10 bar).The results show that the synergy of Ce-O-Pd and Pd-N promotes the formation of active Pd^(δ+),which not only enhances the adsorption of H_(2) and electron-rich C=C bonds,but also contributes to the reduction of proton migration distance and improves proton utilization efficiency.These results provide valuable insights for investigating the regulatory role of the host MOFs,the nature of host-guest interactions,and their correlation with catalytic performance.

Kinetics insights into size effects of carbon nanotubes'growth and their supported platinum catalysts for 4,6-dinitroresorcinol hydrogenation

Size effects are a well-documented phenomenon in heterogeneous catalysis,typically attributed to alterations in geometric and electronic properties.In this study,we investigate the influence of catalyst size in the preparation of carbon nanotube(CNT)and the hydrogenation of 4,6-dinitroresorcinol(DNR)using Fe_(2)O_(3)and Pt catalysts,respectively.Various Fe_(2)O_(3)/Al_(2)O_(3)catalysts were synthesized for CNT growth through catalytic chemical vapor deposition.Our findings reveal a significant influence of Fe_(2)O_(3)nanoparticle size on the structure and yield of CNT.Specifically,CNT produced with Fe_(2)O_(3)/Al_(2)O_(3)containing 28%(mass)Fe loading exhibits abundant surface defects,an increased area for metal-particle immobilization,and a high carbon yield.This makes it a promising candidate for DNR hydrogenation.Utilizing this catalyst support,we further investigate the size effects of Pt nanoparticles on DNR hydrogenation.Larger Pt catalysts demonstrate a preference for 4,6-diaminoresorcinol generation at(100)sites,whereas smaller Pt catalysts are more susceptible to electronic properties.The kinetics insights obtained from this study have the potential to pave the way for the development of more efficient catalysts for both CNT synthesis and DNR hydrogenation.

Novel Method for Evaluating the Aging of Aviation Turbine Engine Oils via High-Temperature Bearing Deposit Tests

Aviation turbine engine oils require excellent thermal-oxidative stability because of their high-temperature environments.High-temperature bearing deposit testing is a mandatory method for measuring the thermal-oxidative performance of aviation lubricant oils,and the relevant apparatus was improved in the present study.Two different commercial aviation turbine engine oils were tested,one with standard performance(known as the SL oil)and the other with high thermal stability,and their thermal-oxidative stability characteristics were evaluated.After 100 h of high-temperature bearing testing,the SL oil was analyzed by using various analytical techniques to investigate its thermal-oxidative process in the bearing test,with its thermal-oxidative degradation mechanism also being discussed.The results indicate that the developed high-temperature bearing apparatus easily meets the test requirements of method 3410.1 in standard FED-STD-791D.The viscosity and total acid number(TAN)of the SL oil increased with the bearing test time,and various deposits were produced in the bearing test,with the micro-particles of the carbon deposits being sphere-like,rod-like,and sheet-like in appearance.The antioxidant additives in the oil were consumed very rapidly in the first 30 h of the bearing test,with N-phenyl-1-naphthylamine being consumed faster than dioctyldiphenylamine.Overall,the oil thermal-oxidative process involves very complex physical and chemical mechanisms.

Inclusion of CoTiO_(3) to ameliorate the re/dehydrogenation properties of the Mg–Na–Al system

For the first time,the MgH_(2)–NaAlH_(4)(ratio 4:1)destabilized system with CoTiO_(3) addition has been explored.The CoTiO_(3)-doped MgH_(2)–NaAlH_(4) sample begins to dehydrogenate at 130℃,which is declined by 40℃ compared to the undoped MgH_(2)–NaAlH_(4).Moreover,the de/rehydrogenation kinetics characteristics of the CoTiO_(3)-doped MgH_(2)–NaAlH_(4) were greatly ameliorated.With the inclusion of CoTiO_(3),the MgH_(2)–NaAlH_(4) composite absorbed 5.2 wt.%H_(2),higher than undoped MgH_(2)–NaAlH_(4).In the context of dehydrogenation,the CoTiO_(3)-doped MgH_(2)–NaAlH_(4) sample desorbed 2.6 wt.%H_(2),almost doubled compared to the amount of hydrogen desorbed from the undoped MgH_(2)–NaAlH_(4) sample.The activation energy obtained by the Kissinger analysis for MgH_(2) decomposition was significantly lower by 35.9 kJ/mol than the undoped MgH_(2)–NaAlH_(4) sample.The reaction mechanism demonstrated that new phases of MgCo and AlTi_(3) were generated in situ during the heating process and are likely to play a substantial catalytic function and be useful in ameliorating the de/rehydrogenation properties of the destabilized MgH_(2)–NaAlH_(4) system with the inclusion of CoTiO_(3).

P-induced electron transfer interaction for enhanced selective hydrogenation rearrangement of furfural to cyclopentanone

Optimizing the intrinsic activity of non-noble metal by precisely tailoring electronic structure offers an appealing way to construct cost-effective catalysts for selective biomass valorization.Herein,we reported a P-doping bifunctional catalyst(Ni-P/mSiO_(2))that achieved 96.6%yield for the hydrogenation rearrangement of furfural to cyclopentanone at mild conditions(1 MPaH_(2),150°C).The turnover frequency of Ni-P/mSiO_(2)was 411.9 h^(-1),which was 3.2-fold than that of Ni/mSiO_(2)(127.2 h^(-1)).Detailed characterizations and differential charge density calculations revealed that the electron-deficient Niδ+species were generated by the electron transfer from Ni to P,which promoted the ring rearrangement reaction.Density functional theory calculations illustrated that the presence of P atoms endowed furfural tilted adsorb on the Ni surface by the C=O group and facilitated the desorption of cyclopentanone.This work unraveled the connection between the localized electronic structures and the catalytic properties,so as to provide a promising reference for designing advanced catalysts for biomass valorization.

High-performance and robust high-temperature polymer electrolyte membranes with moderate microphase separation by implementation of terphenyl-based polymers

Acid loss and plasticization of phosphoric acid(PA)-doped high-temperature polymer electrolyte membranes(HT-PEMs)are critical limitations to their practical application in fuel cells.To overcome these barriers,poly(terphenyl piperidinium)s constructed from the m-and p-isomers of terphenyl were synthesized to regulate the microstructure of the membrane.Highly rigid p-terphenyl units prompt the formation of moderate PA aggregates,where the ion-pair interaction between piperidinium and biphosphate is reinforced,leading to a reduction in the plasticizing effect.As a result,there are trade-offs between the proton conductivity,mechanical strength,and PA retention of the membranes with varied m/p-isomer ratios.The designed PA-doped PTP-20m membrane exhibits superior ionic conductivity,good mechanical strength,and excellent PA retention over a wide range of temperature(80–160°C)as well as satisfactory resistance to harsh accelerated aging tests.As a result,the membrane presents a desirable combination of performance(1.462 W cm^(-2) under the H_(2)/O_(2)condition,which is 1.5 times higher than that of PBI-based membrane)and durability(300 h at 160°C and 0.2 A cm^(-2))in the fuel cell.The results of this study provide new insights that will guide molecular design from the perspective of microstructure to improve the performance and robustness of HT-PEMs.

Silica-modified Pt/TiO_(2) catalysts with tunable suppression of strong metal-support interaction for cinnamaldehyde hydrogenation

Tuning Strong Metal-support Interactions(SMSI)is a key strategy to obtain highly active catalysts,but conventional methods usually enable TiO_(x) encapsulation of noble metal components to minimize the exposure of noble metals.This study demonstrates a catalyst preparation method to modulate a weak encapsulation of Pt metal nanoparticles(NPs)with the supported TiO_(2),achieving the moderate suppression of SMSI effects.The introduction of silica inhibits this encapsulation,as reflected in the characterization results such as XPS and HRTEM,while the Ti^(4+) to Ti^(3+) conversion due to SMSI can still be found on the support surface.Furthermore,the hydrogenation of cinnamaldehyde(CAL)as a probe reaction revealed that once this encapsulation behavior was suppressed,the adsorption capacity of the catalyst for small molecules like H_(2) and CO was enhanced,which thereby improved the catalytic activity and facilitated the hydrogenation of CAL.Meanwhile,the introduction of SiO_(2) also changed the surface structure of the catalyst,which inhibited the occurrence of the acetal reaction and improved the conversion efficiency of C=O and C=C hydrogenation.Systematic manipulation of SMSI formation and its consequence on the performance in catalytic hydrogenation reactions are discussed.