Non-Gaussian quantum states generated via quantum catalysis and their statistical properties

A new kind of non-Gaussian quantum catalyzed state is proposed via multiphoton measurements and two-mode squeezing as an input of thermal state.The characteristics of the generated multiphoton catalysis output state depends on the thermal parameter,catalyzed photon number and squeezing parameter.We then analyze the nonclassical properties by examining the photon number distribution,photocount distribution and partial negativity of the Wigner function.Our findings indicate that nonclassicality can be achieved through the implementation of multiphoton catalysis operations and modulated by the thermal parameter,catalyzed photon number and squeezing parameter.

Cobalt phthalocyanine promoted copper catalysts toward enhanced electro reduction of CO_(2)to C_(2):Synergistic catalysis or tandem catalysis?

The activity and selectivity of electrocatalytic CO_(2)reduction reaction(CO_(2)RR)to C_(2)products on metal catalysts can be regulated by molecular surfactants.However,the mechanism behind it remains elusive and debatable.Herein,copper nanowires(Cu NWs)were fabricated and decorated with cobalt phthalocyanine(CoPc).The electronic interaction between the Cu NWs,CoPc,CO_(2) and CO_(2)RR intermediates were explored by density functional theory(DFT)calculations.It was found that the selectivity and activity of CO_(2)RR towards C_(2)products on Cu NWs were considerably enhanced from 35.2%to 69.9%by surface decoration of CoPc.DFT calculations revealed that CO_(2)RR can proceed in the interphase between Cu substrate and CoPc,and the CO_(2)RR intermediates could synergistically bond with both Cu and Co metal centre in CuNWs-CoPc,which favours the adsorption of CO_(2),CO and CO_(2)RR intermediates,thus reducing the free energy for CO-COcoupling towards C_(2)products.The synergistic interaction was further extended to phthalocyanine(Pc)and other metal phthalocyanine derivatives(MPc),where a relatively weaker synergistic interaction of COintermediates with MPc and Cu substrate and only a slight enhancement of CO_(2)RR towards C_(2) products were observed.This study demonstrates a synergistic catalysis pathway for CO_(2)RR,a novel perspective in interpreting the role of CoPc in enhancing the activity and selectivity of CO_(2)RR on Cu NWs,in contrast to the conventional tandem catalysis mechanism.

Recent advancement and future challenges of photothermal catalysis for VOCs elimination:From catalyst design to applications

Photothermal catalysis realizes the synergistic effect of solar energy and thermochemistry,which also has the potential to improve the reaction rate and optimize the selectivity.In this review,the research progress of photothermal catalytic removal of volatile organic compounds(VOCs)by nano-catalysts in recent years is systematically reviewed.First,the fundamentals of photothermal catalysis and the fabrication of catalysts are described,and the design strategy of optimizing photothermal catalysis performance is proposed.Second,the performance for VOC degradation with photothermal catalysis is evaluated and compared for the batch and continuous systems.Particularly,the catalytic mechanism of VOC oxidation is systematically introduced based on experimental and theoretical study.Finally,the future limitations and challenges have been discussed,and potential research directions and priorities are highlighted.A broad view of recent photothermal catalyst fabrication,applications,challenges,and prospects can be systemically provided by this review.

Effects of Catalysis and Separator Functionalization on High-Energy Lithium–Sulfur Batteries:A Complete Review

Lithium–sulfur(Li-S)batteries have the advantages of high theoretical specific capacity(1675 mAh g^(−1)),rich sulfur resources,low production cost,and friendly environment,which makes it one of the most promising next-generation rechargeable energy storage devices.However,the“shuttle effect”of polysulfide results in the passivation of metal lithium anode,the decrease of battery capacity and coulombic efficiency,and the deterioration of cycle stability.To realize the commercialization of Li-S batteries,its serious“shuttle effect”needs to be suppress.The commercial separators are ineffective to suppress this effect because of its large pore size.Therefore,it is an effective strategy to modify the separator surface and introduce functional modified layer.In addition to the blocking strategy,the catalysis of polysulfide conversion reaction is also an important factor hindering the migration of polysulfides.In this review,the principles of separator modification,functionalization,and catalysis in Li-S batteries are reviewed.Furthermore,the research trend of separator functionalization and polysulfide catalysis in the future is prospected.

Sustainable Ammonia Synthesis from Nitrogen and Water by One-Step Plasma Catalysis

Sustainable ammonia synthesis at ambient conditions that relies on renewable sources of energy and feedstocks is globally sought to replace the Haber-Bosch process.Here,using nitrogen and water as raw materials,a nonthermal plasma catalysis approach is demonstrated as an effective powerto-chemicals conversion strategy for ammonia production.By sustaining a highly reactive environment,successful plasma-catalytic production of NH_(3) was achieved from the dissociation of N_(2) and H_(2)O under mild conditions.Plasma-induced vibrational excitation is found to decrease the N_(2) and H_(2)O dissociation barriers,with the presence of matched catalysts in the nonthermal plasma discharge reactor contributing significantly to molecular dissociation on the catalyst surface.Density functional theory calculations for the activation energy barrier for the dissociation suggest that ruthenium catalysts supported on magnesium oxide exhibit superior performance over other catalysts in NH_(3) production by lowering the activation energy for the dissociative adsorption of N_(2) down to 1.07 eV.The highest production rate,2.67 mmol gcat.^(-1) h^(-1),was obtained using ruthenium catalyst supported on magnesium oxide.This work highlights the potential of nonthermal plasma catalysis for the activation of renewable sources to serve as a new platform for sustainable ammonia production.

Design of ZnSe-CoSe heterostructure decorated in hollow N-doped carbon nanocage with generous adsorption and catalysis sites for the reversibly fast kinetics of polysulfide conversion

Although lithium-sulfur batteries(Li SBs)are regarded as one of the most promising candidates for the next-generation energy storage system,the actual industrial application is hindered by the sluggish solid–liquid phase conversion kinetics,severe shuttle effect,and low sulfur loadings.Herein,a zeolitic imidazolate framework(ZIF)derived heterogeneous ZnSe-CoSe nanoparticles encapsulated in hollow N-doped carbon nanocage(ZnSe-CoSe-HNC)was designed by etching with tannic acid as a multifunctional electrocatalyst to boost the polysulfide conversion kinetics in LiSBs.The hollow structure in ZIF ensures large inner voids for sulfur and buffering volume expansions.Abundant exposed ZnSe-CoSe heterogeneous interfaces serve as bifunctional adsorption-catalytic centers to accelerate the conversion kinetics and alleviate the shuttle effect.Together with the highly conductive framework,the ZnSe-CoSeHNC/S cathode exhibits a high initial reversible capacity of 1305.3 m A h g-1at 0.2 C,high-rate capability,and reliable cycling stability under high sulfur loading and lean electrolyte(maintaining at 745 m A h g-1after 200 cycles with a high sulfur loading of 6.4 mg cm-2and a low electrolyte/sulfur ratio of 6μL mg^(-1)).Theoretical calculations have demonstrated the heterostructures of ZnSe-CoSe offer higher binding energy to lithium polysulfides than that of ZnSe or CoSe,facilitating the electron transfer to lithium polysulfides.This work provides a novel heterostructure with superior catalytic ability and hollow conductive architecture,paving the way for the practical application of functional sulfur electrodes.

Designing high-efficiency light-to-thermal conversion materials for solar desalination and photothermal catalysis

Light-to-thermal conversion materials(LTCMs)have been of great interest to researchers due to their impressive energy conversion capacity and wide range of applications in biomedical,desalination,and synergistic catalysis.Given the limited advances in existing materials(metals,semiconductors,π-conjugates),researchers generally adopt the method of constructing complex systems and hybrid structures to optimize performance and achieve multifunctional integration.However,the development of LTCMs is still in its infancy as the physical mechanism of light-to-thermal conversion is unclear.In this review,we proposed design strategies for efficient LTCMs by analyzing the physical process of light-tothermal conversion.First,we analyze the nature of light absorption and heat generation to reveal the physical processes of light-to-thermal conversion.Then,we explain the light-to-thermal conversion mechanisms of metallic,semiconducting andπ-conjugated LCTMs,and propose new material design strategies and performance improvement methods.Finally,we summarize the challenges and prospects of LTCMs in emerging applications such as solar water evaporation and photothermal catalysis.

Tandem catalysis for enhanced CO oxidation over the Bi-Au-SiO_(2)interface

Bimetallic catalysts typically exploit unique synergetic effects between two metal species to achieve their catalytic effect.Understanding the mechanism of CO oxidation using hybrid heterogeneous catalysts is important for effective catalyst design and environmental protection.Herein,we report a Bi-Au/SiO_(2)tandem bimetallic catalyst for the oxidation of CO over the Au/SiO_(2)surface,which was monitored using near-ambient-pressure X-ray photoelectron spectroscopy.The Au-decorated SiO_(2)catalyst exhibited scarce activity in the CO oxidation reaction;however,the introduction of Bi to the Au/SiO_(2)system promoted the catalytic activity.The mechanism is thought to involve the dissociation O_(2)molecules in the presence of Bi,which results in spillover of the O species to adjacent Au atoms,thereby forming Au^(δ+).Further CO adsorption,followed by thermal treatment,facilitated the oxidation of CO at the Au-Bi interface,resulting in a reversible reversion to the neutral Au valence state.Our work provides insight into the mechanism of CO oxidation on tandem surfaces and will facilitate the rational design of other Au-based catalysts.

Cooperative catalysis of Co single atoms and nanoparticles enables selective CAr-OCH_(3) cleavage for sustainable production of lignin-based cyclohexanols

In this work,a dual-size MOF-derived Co catalyst(0.2Co_(1-NPs)@NC)composed of single atoms(Co_(1))and highly dispersed nanoparticles(Co NPs)was prepared by in-situ Zn evaporation for the highperformance conversion of lignin-derived o-methoxyphenols(lignin oil)to cyclohexanols(up to 97%yield)via cascade demethoxylation and dearomatization.Theoretical calculations elaborated that the dual-size Co catalyst exhibited a cooperative effect in the selective demethoxylation process,in which the Co NPs could initially dissociate hydrogen at lower energies while Co1remarkably facilitated the cleavage of the C_(Ar)-OCH_(3)bond.Moreover,the intramolecular hydrogen bonds formed in the omethoxy-containing phenols were found to result in a decrease in the bond energy of the C_(Ar)-OCH_(3)bond,which was more prone to be activated by the dual-size Co sites.Notably,the pre-hydrogenated intermediate(e.g.,2-methoxycyclohexanol from guaiacol)is difficult to undergo demethoxylation,indicating that the selective C_(Ar)-OCH_(3)bond cleavage is a prerequisite for the synthesis of cyclohexanols.The 0.2Co_(1-NPs)@NC catalyst was highly recyclable with a neglect decline in activity during five consecutive cycles.This cooperative catalytic strategy based on the metal size effect opens new avenues for biomass upgrading via enhanced C-O bond cleavage of high selectivity.

Is a catalyst always beneficial in plasma catalysis? Insights from the many physical and chemical interactions

Plasma-catalytic dry reforming of CH_(4)(DRM) is promising to convert the greenhouse gasses CH_(4) and CO_(2) into value-added chemicals, thus simultaneously providing an alternative to fossil resources as feedstock for the chemical industry. However, while many experiments have been dedicated to plasma-catalytic DRM, there is no consensus yet in literature on the optimal choice of catalyst for targeted products,because the underlying mechanisms are far from understood. Indeed, plasma catalysis is very complex,as it encompasses various chemical and physical interactions between plasma and catalyst, which depend on many parameters. This complexity hampers the comparison of experimental results from different studies, which, in our opinion, is an important bottleneck in the further development of this promising research field. Hence, in this perspective paper, we describe the important physical and chemical effects that should be accounted for when designing plasma-catalytic experiments in general, high-lighting the need for standardized experimental setups, as well as careful documentation of packing properties and reaction conditions, to further advance this research field. On the other hand, many parameters also create many windows of opportunity for further optimizing plasma-catalytic systems.Finally, various experiments also reveal the lack of improvement in plasma catalysis compared to plasma-only, specifically for DRM, but the underlying mechanisms are unclear. Therefore, we present our newly developed coupled plasma-surface kinetics model for DRM, to provide more insight in the underlying reasons. Our model illustrates that transition metal catalysts can adversely affect plasmacatalytic DRM, if radicals dominate the plasma-catalyst interactions. Thus, we demonstrate that a good understanding of the plasma-catalyst interactions is crucial to avoiding conditions at which these interactions negatively affect the results, and we provide some recommendations for improvement. For instance, we believe that plasma-catalytic DRM may benefit more from higher reaction temperatures,at which vibrational excitation can enhance the surface reactions.

The Nature of Active Sites for Plasmon-Mediated Photothermal Catalysis and Heat-Coupled Photocatalysis in Dry Reforming of Methane

Solar energy-induced catalysis has been attracting intensive interests and its quantum efficiencies in plasmon-mediated photothermal catalysis(P-photothermal catalysis)and external heat-coupled photocatalysis(E-photothermal catalysis)are ultimately determined by the catalyst structure for photo-induced energetic hot carriers.Herein,different catalysts of supported(TiO_(2)-P25 and Al_(2)O_(3))platinum quantum dots are employed in photo,thermal,and photothermal catalytic dry reforming of methane.Integrated experimental and computational results unveil different active sites(hot zones)on the two catalysts for photo,thermal,and photothermal catalysis.The hot zones of P-photothermal catalysis are identified to be the metal-support interface on Pt/P25 and the Pt surface on Pt/Al_(2)O_(3),respectively.However,a change of the active site to the Pt surface on Pt/P25 is for the first time observed in E-photothermal catalysis(external heating temperature of 700℃).The hot zones contribute to the significant enhancements in photothermal catalytic reactivity against thermocatalysis.This study helps to understand the reaction mechanism of photothermal catalysis to exploit efficient catalysts for solar energy utilization and fossil fuels upgrading.

Ti-Fe_(2)O_(3)/Ni(OH)_(x) as an efficient and durable photoanode for the photoelectrochemical catalysis of PET plastic to formic acid

Photoelectrochemical(PEC) technology provides a promising prospect for the transformation of polyethylene terephthalate(PET) plastic wastes to produce value-added chemicals.The PEC catalytic systems with high activity,selectivity and long-term durability are required for the future up-scaling industrial applications.Herein,we employed the interfacial modification strategy to develop an efficient and stable photoanode and evaluated its PEC activity for ethylene glycol(EG,derived from PET hydrolysate) oxidation to formic acid.The interfacial modification between Fe_(2)O_(3)semiconductor and Ni(OH)xcocatalyst with ultrathin TiO_(x) interlayer not only improved the photocurrent density by accelerating the kinetics of photogenerated charge carriers,but also kept the high Faradaic efficiency(over 95% in 30 h) towards the value-added formic acid product.This work proposes an effective method to promote the PEC activity and enhance the long-term stability of photoelectrodes for upcycling PET plastic wastes.

Review on Metal-Acid Tandem Catalysis for Hydrogenative Rearrangement of Furfurals to C_(5) Cyclic Compounds

Hydrogenative rearrangement of biomas s-derived furfurals(furfural and 5-hydroxymethyl furfural) to C_(5) cyclic compounds(such as cyclopentanones and cyclopentanols) offers an expedient reaction route for acquiring O-containing value-added chemicals thereby replacing the traditional petroleum-based approaches.The scope for developing efficient bifunctional catalysts and establishing mild reaction conditions for upgrading furfurals to cyclic compounds has stimulated immense deliberation in recent years.Extensive efforts have been made toward developing catalysts for multiple tandem conversions,including those with various metals and supports.In this scientific review,we aim to summarize the research progress on the synergistic effect of the metal-acid sites,including simple metal-supported acidic supports,adjacent metal acid sites-supported catalysts,and in situ H_(2)-modified bifunctional catalysts.Distinctively,the catalytic performance,catalytic mechanism,and future challenges for the hydrogenative rearrangement are elaborated in detail.The methods highlighted in this review promote the development of C_(5) cyclic compound synthesis and provide insights to regulate bifunctional catalysis for other applications.

Research on the Construction of Industrial Catalysis Course Under the Background of Specialty-Innovation Integration

“Specialty-innovation integration”is a positive response of higher education to economic and social development needs,and it is also an inherent requirement for the reform and development of higher education.This paper discusses the construction of an“industrial catalysis”curriculum system under the background of specialty-innovation integration.Overall,it raises students’comprehensive quality from three aspects,including teaching content,teaching method,and the concept of specialty-innovation integration,aiming to cultivate students as the innovative talents required by the development of the era for national and regional development.

基于Catalysis的面向构件建模方法研究

介绍了基于Catalysis应用面向构件建模方法进行系统分析、设计、建立系统模型的简洁方法。通过对集团型全面预算管理系统的建模过程,给出了该方法的应用细节,将基于构件的软件开发和企业级应用的特点结合起来,给基于分层结构的企业级软件系统的开发以明确的指导。

Chlorobenzene degradation by electro-heterogeneous catalysis in aqueous solution:intermediates and reaction mechanism

This study was performed to investigate the variables that influence chlorobenzene (CB) degradation in aqueous solution by electro-heterogeneous catalysis.The effects of current density,pH,and electrolyte concentration on CB degradation were determined.The degradation effciency of CB was almost 100% with an initial CB concentration of 50 mg/L,current density 15 mA/cm2,initial pH 10,electrolyte concentration 0.1 mol/L,and temperature 25°C after 90 min of reaction.Under the same conditions,the degradation eff...

Cooperation of nitrogen-doping and catalysis to improve the Li-ion storage performance of lignin-based hard carbon

Hard carbon draws great interests as anode material in lithium ion batteries （LIBs） due to its high the- oretical capacity, high rate capability and abundance of its precursors. Herein we firstly synthesize the lignin-melamine resins by grafting melamine onto lignin. Afterwards, nitrogen doped hard carbon is pre- pared by the pyrolysis of lignin-melamine resins with the aid of catalyst （Ni（NO_3）2·6H_2O） at 1000 ℃. Compared with the samples without nitrogen-doping and catalysis, as-prepared nitrogen doped hard car- bon exhibits higher reversible capacity （345 mAh g-1 at 0.1 A g-1 ）, higher rate capability （145 mAh g-1 at 5 A g-1） and excellent cycling stability. The superior electrochemical performance is ascribed to the synergistic effect of nitrogen doping, graphitic structure and amorphous structure. Among them, nitro- gen doping could create the vacancies around the nitrogen sites, which enhance the reactivity and the electronic conductivity of materials. Additionally, graphitic structure also enhances the electronic con- ductivity of materials, thus improving the electrochemical performance of hard carbon. It is worthwhile that Iignin, renewable and abundant biopolymer, is converted to hard carbon with good electrochemical performance, which realizes the high value utilization of lignin.

Catalysis Conversion Methane into C_(2) Hydrocarbons via Electric Field Enhanced Plasma

In this paper the effect of catalyst and carrier in electric field enhanced plasma on methane conversion into C2 hydrocarbons was investigated. Methane coupling reaction was studied in the system of continuous flow reactor on Ni, MoO3, MnO2 catalysts and different ZSM-5 carriers. The per pass conversion of methane can be as high as 22%, the selectivity of ethylene can be as high as 23.8%, of acetylene 60.8%, of ethane 5.4% and of total C2 hydrocarbons was more than 90%. ZSM-5-25 was the better carrier and MnO2 was the better active component. The efficiency of energy was as high as 7.81%.

K_2CO_3 catalysis on the reactivity of top charged coke and stamp charged coke

The catalysis of K2CO3 on the reactivity of top charged coke and stamp charged coke from Pansteel in China was studied. The coke reaction index of the stamp charged coke was 1%-2% higher than that of the top charged coke. Under the catalysis of K2CO3, the coke reaction index of both cokes approximately increased by 4%, 6%, 10% and 6% at 900, 1000, 1100 and 1200℃, respectively. The reactivity of the K-enriched stamp charged coke was 1%-2% higher than that of the K-enriched top charged coke below 1100℃. However, only negligible differences were found in the temperature zone between 1100 and 1200℃. Scanning electron microscopy images illustrated that pores in the top charged coke were smaller and equally distributed, while relatively more big pores exist non-homogenously in stamp charged coke. Due to the different processes in production, the stamp charged coke was more porous and most of the pores tended to be applanate. Cracks were observed in the microstructure of the stamp charged coke during the carbon solution reaction, implying the inferior quality of the stamp charged coke to the top charged coke at high temperature. Diffusion of K during the carbon solution reaction was studied by the energy dispersive spectrometry. It is found that K gradually spreads into the center of lumpy coke with the rising of temperature and is equally distributed on the edges of pores at 1200℃. Besides, oxidation reactions of functional groups become faster with the catalysis of K.content

Destruction of VOCs by combination of corona discharge and catalysis techniques

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