New ternary superconducting compound LaRu2As2： Physical properties from density functional theory calculations

In this paper, we perform the density functional theory(DFT)-based calculations by the first-principles pseudopotential method to investigate the physical properties of the newly discovered superconductor LaRu_2As_2 for the first time.The optimized structural parameters are in good agreement with the experimental results. The calculated independent elastic constants ensure the mechanical stability of the compound. The calculated Cauchy pressure, Pugh's ratio as well as Poisson's ratio indicate that LaRu_2As_2 should behave as a ductile material. Due to low Debye temperature, LaRu_2As_2 may be used as a thermal barrier coating(TBC) material. The new compound should exhibit metallic nature as its valence bands overlap considerably with the conduction bands. LaRu_2As_2 is expected to be a soft material and easily machinable because of its low hardness value of 6.8 GPa. The multi-band nature is observed in the calculated Fermi surface. A highly anisotropic combination of ionic, covalent and metallic interactions is expected to be in accordance with charge density calculation.

Design of high-performance ion-doped CoP systems for hydrogen evolution:From multi-level screening calculations to experiment

Rational design of high-performance electrocatalysts for hydrogen evolution reaction(HER)is vital for future renewable energy systems.The incorporation of foreign metal ions into catalysts can be an effective approach to optimize its performance.However,there is a lack of systematic theoretical studies to reveal the quantitative relationships at the electronic level.Here,we develop a multi-level screening methodology to search for highly stable and active dopants for CoP catalysts.The density functional theory(DFT)calculations and symbolic regression(SR)were performed to investigate the relationship between the adsorption free energy(ΔG_(H^(*)))and 10 electronic parameters.The mathematic formulas derived from SR indicate that the difference of work function(ΔΦ)between doped metal and the acceptor plays the most important role in regulatingΔG_(H^(*)),followed by the d-band center(d-BC)of doped system.The descriptor of HER can be expressed asΔG_(H^(*))=1.59×√|0.188ΔΦ+d BC+0.120|1/2-0.166 with a high determination coefficient(R^(2)=0.807).Consistent with the theoretical prediction,experimental results show that the Al-CoP delivers superior electrocatalytic HER activity with a low overpotential of75 m V to drive a current density of 10 mA cm^(-2),while the overpotentials for undoped CoP,Mo-CoP,and V-CoP are 206,134,and 83 m V,respectively.The current work proves that theΔΦis the most significant regulatory parameter ofΔG_(H^(*))for ion-doped electrocatalysts.This finding can drive the discovery of high-performance ion-doped electrocatalysts,which is crucial for electrocatalytic water splitting.

Active MoS_(2)-based electrode for green ammonia synthesis

Nitrogen electro-reduction under mild conditions is one promising alternative approach of the energyconsuming Haber-Bosch process for the artificial ammonia synthesis.One critical aspect to unlocking this technology is to discover the catalysts with high selectivity and efficiency.In this work,the N_(2)-to-NH_(3)conversion on the functional MoS_(2)is fully investigated by density functional theory calculations since the layered MoS_(2)provides the ideal platform for the elaborating copies of the nitrogenase found in nature,wherein the functionalization is achieved via basal-adsorption,basal-substitution or edge-substitution of transition metal elements.Our results reveal that the edge-functionalization is a feasible strategy for the activity promotion;however,the basal-adsorption and basal-substitution separately suffer from the electrochemical instability and the NRR inefficiency.Specifically,MoS_(2)functionalized via edge W-substitution exhibits an exceptional activity.The energetically favored reaction pathway is through the distal pathway and a limiting potential is less than 0.20 V.Overall,this work escalates the rational design of the high-effective catalysts for nitrogen fixation and provides the explanation why the predicated catalyst have a good performance,paving the guidance for the experiments.

Engineering Two-Phase Bifunctional Oxygen Electrocatalysts with Tunable and Synergetic Components for Flexible Zn-Air Batteries

Metal-air batteries,like Zn-air batteries(ZABs)are usually suffered from low energy conversion efficiency and poor cyclability caused by the sluggish OER and ORR at the air cathode.Herein,a novel bimetallic Co/CoFe nanomaterial supported on nanoflower-like N-doped graphitic carbon(NC)was prepared through a strategy of coordination construction-cation exchange-pyrolysis and used as a highly efficient bifunctional oxygen electrocatalyst.Experimental characterizations and density functional theory calculations reveal the formation of Co/CoFe heterostructure and synergistic effect between metal layer and NC support,leading to improved electric conductivity,accelerated reaction kinetics,and optimized adsorption energy for intermediates of ORR and OER.The Co/CoFe@NC exhibits high bifunctional activities with a remarkably small potential gap of 0.70 V between the half-wave potential(E_(1/2))of ORR and the potential at 10 mA cm^(-2)(E_(j=10))of OER.The aqueous ZAB constructed using this air electrode exhibits a slight voltage loss of only 60 mV after 550-cycle test(360 h,15 days).A sodium polyacrylate(PANa)-based hydrogel electrolyte was synthesized with strong water-retention capability and high ionic conductivity.The quasi-solid-state ZAB by integrating the Co/CoFe@NC air electrode and PANa hydrogel electrolyte demonstrates excellent mechanical stability and cyclability under different bending states.

Mg/Fe site-specific dual-doping to boost the performance of cobalt-free nickle-rich layered oxide cathode for high-energy lithium-ion batteries

Layer-type LiNi0.9Mn0.1O2is promising to be the primary cathode material for lithium-ion batteries(LIBs)due to its excellent electrochemical performance.Unfortunately,the cathode with high nickel content suffers from severely detrimental structural transformation that causes rapid capacity attenuation.Herein,site-specific dual-doping with Fe and Mg ions is proposed to enhance the structural stability of LiNi0.9Mn0.1O2.The Fe3+dopants are inserted into transition metal sites(3b)and can favorably provide additional redox potential to compensate for charge and enhance the reversibility of anionic redox.The Mg ions are doped into the Li sites(3a)and serve as O_(2)^(-)-Mg^(2+)-O_(2)^(-)pillar to reinforce the electrostatic cohesion between the two adjacent transition-metal layers,which further suppress the cracking and the generation of harmful phase transitions,ultimately improving the cyclability.The theoretical calculations,including Bader charge and crystal orbital Hamilton populations(COHP)analyses,confirm that the doped Fe and Mg can form stable bonds with oxygen and the electrostatic repulsion of O_(2)^(-)-O_(2)^(-)can be effectively suppressed,which effectively mitigates oxygen anion loss at the high delithiation state.This dual-site doping strategy offers new avenues for understanding and regulating the crystalline oxygen redox and demonstrates significant potential for designing high-performance cobalt-free nickel-rich cathodes.

Exploring the mechanism of Ta_(3)N_(5)/KTaO_(3) photocatalyst for overall water splitting by first-principles calculations

The rational fabrication of heterostructures is one of efficient strategies for improving photocatalytic performance of semiconductor photocatalysts.Very recently,Domen and co-workers found that Ta_(3)N_(5) single crystals grown on the surface of KTaO_(3) can accomplish photocatalytic overall water splitting for the first time.In order to comprehend the underlying mechanism of this photocatalytic system,we have performed a systematic study based on density functional theory first-principles calculations.Ta_(3)N_(5)(010)/KTaO_(3)(110)slab models have been built according to experimental observations by considering two common terminations of KTaO_(3)(110)surface,named as Ta_(3)N_(5)/O_(2) and Ta_(3)N_(5)/KTaO.The formations of interfacial bonds are thermodynamically stable,showing a covalent interaction between two components of a heterostructure.Ta_(3)N_(5)/O_(2) has a higher mobility of photogenerated charge carriers and lower recombination rate of charge carriers than Ta_(3)N_(5)/KTaO.The light absorption of heterostructures displays the feature of KTaO_(3) in the short wavelength region and the characteristic of Ta_(3)N_(5) in the long wavelength region.The calculated band offsets show that Ta_(3)N_(5)/O_(2) and Ta_(3)N_(5)/KTaO have distinct Type-II band alignments,with Ta_(3)N_(5) as the accumulator of photoinduced electrons in the former and the collector of photogenerated holes in the latter,respectively.The difference in charge density and electrostatic potential between two components acts as a driving force to promote the transfer of electrons and holes to different domains of the interface,which is beneficial to extend the lifetime of photoinduced carriers.Our results demonstrate that the function of Ta_(3)N_(5) in Ta_(3)N_(5)/KTaO_(3) photocatalytic system is determined by the termination property of KTaO_(3)(110)surface,which provides a likely reason of the observed photocatalytic activity of overall water splitting achieved by Ta_(3)N_(5) synthesized by using KTaO_(3) as a precursor for the nitridation reaction.

The role of copper in enhancing the performance of heteronuclear diatomic catalysts for the electrochemical CO_(2)conversion to C_(1) chemicals

Diatomic catalysts(DACs)with two adjacent metal atoms supported on graphene can offer diverse functionalities,overcoming the inherent limitations of single atom catalysts(SACs).In this study,density functional theory calculations were conducted to investigate the reactivity of the carbon dioxide(CO_(2))reduction reaction(CO_(2)RR)on metal sites of both DACs and SACs,as well as their synergistic effects on activity and selectivity.Calculation of the Gibbs free energies of CO_(2)RR and associated values of the limiting potentials to generate C_(1) products showed that Cu acts as a promoter rather than an active catalytic centre in the catalytic CO_(2)conversion on heteronuclear DACs(CuN_(4)-MN_(4)),improving the catalytic activity on the other metal compared to the related SAC MN_(4).Cu enhances the initial reduction of CO_(2)by promoting orbital hybridization between the key intermediate*COOH 2p-orbitals and the metals 3d-orbitals around the Fermi level.This degree of hybridization in the DACs CuN_(4)-MN_(4) decreases from Fe to Co,Ni,and Zn.Our work demonstrates how Cu regulates the CO_(2)RR performance of heteronuclear DACs,offering an effective approach to designing practical,stable,and high-performing diatomic catalysts for CO_(2)electroreduction.

Introducing oxygen vacancies in TiO_(2) lattice through trivalent iron to enhance the photocatalytic removal of indoor NO

The synthesis of oxygen vacancies(OVs)-modified TiO_(2)under mild conditions is attractive.In this work,OVs were easily introduced in TiO_(2)lattice during the hydrothermal doping process of trivalent iron ions.Theoretical calculations based on a novel charge-compensation structure model were employed with experimental methods to reveal the intrinsic photocatalytic mechanism of Fe-doped TiO_(2)(Fe-TiO_(2)).The OVs formation energy in Fe-TiO_(2)(1.12 eV)was only 23.6%of that in TiO_(2)(4.74 eV),explaining why Fe^(3+)doping could introduce OVs in the TiO_(2)lattice.The calculation results also indicated that impurity states introduced by Fe^(3+)and OVs enhanced the light absorption activity of TiO_(2).Additionally,charge carrier transport was investigated through the carrier lifetime and relative mass.The carrier lifetime of Fe-TiO_(2)(4.00,4.10,and 3.34 ns for 1at%,2at%,and 3at%doping contents,respectively)was longer than that of undoped TiO_(2)(3.22 ns),indicating that Fe^(3+) and OVs could promote charge carrier separation,which can be attributed to the larger relative effective mass of electrons and holes.Herein,Fe-TiO_(2)has higher photocatalytic indoor NO removal activity compared with other photocatalysts because it has strong light absorption activity and high carrier separation efficiency.

Study of engineering electronic structure modulated non-noble metal oxides for scaled-up alkaline blend seawater splitting

Scaled-up industrial water electrolysis equipment that can be used with abundant seawater is key for affordable hydrogen production.The search for highly stable,dynamic,and economical electrocatalysts could have a significant impact on hydrogen commercialization.Herein,we prepared energy-efficient,scalable,and engineering electronic structure modulated Mn-Ni bimetal oxides(Mn_(0.25)Ni_(0.75)O)through simple hydrothermal followed by calcination method.As-optimized Mn_(0.25)Ni_(0.75)O displayed enhanced oxygen and hydrogen evolution reaction(OER and HER)performance with overpotentials of 266 and115 mV at current densities of 10 mA cm^(-2)in alkaline KOH added seawater electrolyte solution.Additionally,Mn-Ni oxide catalytic benefits were attributed to the calculated electronic configurations and Gibbs free energy for OER,and HER values were estimated using first principles calculations.In real-time practical application,we mimicked industrial operating conditions with modified seawater electrolysis using Mn_(0.25)Ni_(0.75)O‖Mn_(0.25)Ni_(0.75)O under various temperature conditions,which performs superior to the commercial IrO_(2)‖Pt-C couple.These findings demonstrate an inexpensive and facile technique for feasible large-scale hydrogen production.

Density Functional Theory Study on the Complete Substitutions of Nd and Fe by Other Rare-earth and Transition-metal Elements in Nd_(2)Fe_(14)B Compound

To search for proper alternatives to improve the magnetic properties of Nd_(2)Fe_(14)B,using first-principles density functional theory calculations we have systematically studied the R_(2)M_(14)B(R=lanthanides from La to Lu;M=Mn,Fe,Co,and Ni)compounds with the isomorphic structure of Nd_(2)Fe_(14)B.The results show that for rare-earth elements,Pr is the most suitable choice for considering as an alternative of Nd.As for the substitution of Fe in Nd_(2)Fe_(14) B by other transition-metal elements,Co is much more suitable than Mn and Ni because the latter two result in too significant reduction of the magnetic moment.

Single‐atomic Co‐B_(2)N_(2)sites anchored on carbon nanotube arrays promote lithium polysulfide conversion in lithium-sulfur batteries

Due to low cost,high capacity,and high energy density,lithium–sulfur(Li–S)batteries have attracted much attention;however,their cycling performance was largely limited by the poor redox kinetics and low sulfur utilization.Herein,predicted by density functional theory calculations,single‐atomic Co‐B2N2 site‐imbedded boron and nitrogen co‐doped carbon nanotubes(SA‐Co/BNC)were designed to accomplish high sulfur loading,fast kinetic,and long service period Li–S batteries.Experiments proved that Co‐B2N2 atomic sites can effectively catalyze lithium polysulfide conversion.Therefore,the electrodes delivered a specific capacity of 1106 mAh g−1 at 0.2 C after 100 cycles and exhibited an outstanding cycle performance over 1000 cycles at 1 C with a decay rate of 0.032%per cycle.Our study offers a new strategy to couple the combined effect of nanocarriers and single‐atomic catalysts in novel coordination environments for high‐performance Li–S batteries.

Li_(2)TiO_(3) Dopant and Phosphate Coating Improve the Electrochemical Performance of LiCoO2 at 3.0-4.6 V

A sol-gel tandem with a solid-phase modification procedure was developed to synthesize Li_(2)TiO_(3)-doped LiCoO_(2) together with phosphate coatings(denoted as LCO-Ti/P),which possesses excellent high-voltage performance in the range of 3.0-4.6 V.The characterizations of X-ray diffraction,high-resolution transmission electron microscopy,and X-ray photoelectron spectroscopy illustrated that the modified sample LCO-Ti/P had the dopant of monoclinic Li_(2)TiO_(3) and amorphous Li3PO4 coating layers.LCO-Ti/P has an initial discharge capacity of 211.6 mAh/g at 0.1 C and a retention of 85.7%after 100 cycles at 1 C and 25±1°C between 3.0 and 4.6 V.Nyquist plots reflect that the charge transfer resistance of LCO-Ti/P after 100 cycles at 1 C is much lower than that of the spent LCO,which benefits Li-ion diffusion.Density functional theory calculations disclose the superior lattice-matching property of major crystal planes for Li_(2)TiO_(3) and LiCoO_(2),the lower energy barriers for Li-ion diffusion in Li_(2)TiO_(3),and the suppressed oxygen release performance resulting from phosphate adsorption.This work provides useful guidance on the rational design of the high-voltage performance of modified LiCoO_(2) materials in terms of lattice-matching properties aside from the phosphate coating to reduce the energy barriers of Li-ion diffusion and enhance cycling stability.

Density functional theory study on the role of ternary alloying elements in TiFe-based hydrogen storage alloys

The role of additional ternary alloying elements on the performance of stationary TiFe-based hydrogen storage alloys was investigated based on first-principles density functional theory calculations.As a basic step for examinations,the site preference of each alloying element in the stoichiometric and nonstoichiometric B2TiFe compounds was clarified considering possible antisite defects.Based on the revealed site preference,the effect of various possible ternary elements on the hydrogen storage was examined by focusing on the formation enthalpies of TiFeH and TiFeH_(2) hydrides,which were closely related to the change in the location of plateaus in the pressure-composition-temperature curve.Several physical properties such as the volume expansion due to hydride formation were also examined to provide additional criteria for selecting optimum alloying conditions in future alloying design processes.Candidate alloying elements that maximize the grain boundary embrittlement due to the solute segregation were proposed for the enhanced initial activation of TiFe-based hydrogen storage alloys.

Defective ZnS nanoparticles anchored in situ on N-doped carbon as a superior oxygen reduction reaction catalyst

Defect engineering has been used to develop low-cost and effective catalysts to boost oxygen reduction reactions.However,the development of catalysts that use metal cation vacancies as the active sites for oxygen reduction reaction is lacking.In this study,ZnS nanoparticles on N-doped carbon serve as an oxygen reduction reaction catalyst.These catalysts were prepared via a one-step method at 900℃.Amazingly,the high-resolution transmission electron microscope image revealed obvious defects in the ZnS nanoparticles.These facilitated the catalyst synthesis,and the product displayed good electrocatalytic performance for the oxygen reduction reaction in an alkaline medium,including a lower onset potential,lower mid-wave potential,four electron transfer process,and better durability compared with 20 wt%Pt/C.More importantly,the density functional theory results indicated that using the Zn vacancies in the prepared catalyst as active sites required a lower reaction energy to produce OOH*from*OO toward oxygen reduction reaction.Therefore,the proposed catalyst with Zn vacancies can be used as a potential electrocatalyst and may be substitutes for Pt-based catalysts in fuel cells,given the novel catalyst’s resulting performance.

Incorporation of layered tin(Ⅳ) phosphate in graphene framework for high performance lithium-sulfur batteries

To anchor the polysulfide and enhance the conversion kinetics of polysulfide to disulfide/sulfide is critical for improving the performance of lithium-sulfur battery.For this purpose,the graphene-supported tin(Ⅳ) phosphate(Sn(HPO_4)_2·H_2 O,SnP) composites(SnP-G) are employed as the novel sulfur hosts in this work.When compared to the graphene-sulfur and carbon-sulfur composites,the SnP-G-sulfur composites exhibit much better cycling performance at 1.0 C over 800 cycles.Meanwhile,the pouch cell fabricated with the SnP-G-sulfur cathodes also exhibits excellent performance with an initial capacity of1266.6 mAh g^(-1)(S) and capacity retention of 76.9% after 100 cycles at 0.1 C.The adsorption tests,density functional theory(DFT) calculations in combination with physical cha racterizations and electrochemical measurements provide insights into the mechanism of capture-accelerated conversion mechanism of polysulfide at the surface of SnP.DFT calculations indicate that the Li-O bond formed between Li atom(from Li_2 S_n,n=1,2,4,6,8) and O atom(from PO_3-OH in SnP) is the main reason for the strong interactions between Li_2 S_n and SnP.As a result,SnP can effectively restrain the shuttle effect and improving the cycling performance of Li-S cell.In addition,by employing the climbing-image nudged elastic band(ciNEB) methods,the energy barrier for lithium sulfide decomposition(charging reaction) on SnP is proved to decrease significantly compared to that on graphene.It can be concluded that SnP is an effective sulfur hosts acting as dual-functional accelerators for the conversion reactions of polysulfude to sulfide(discharging reaction) as well as polysulfide to sulfur(charging reaction).

Mg-intercalation engineering of MnO_(2)electrode for high-performance aqueous magnesium-ion batteries

Rechargeable aqueous magnesium-ion batteries(MIBs)show great promise for low-cost,high-safety,and high-performance energy storage applications.Although manganese dioxide(MnO_(2))is considered as a potential electrode material for aqueous MIBs,the low electrical conductivity and unsatisfactory cycling performance greatly hinder the practical application of MnO_(2)electrode.To overcome these problems,herein,a novel Mg-intercalation engineering approach for MnO_(2)electrode to be used in aqueous MIBs is presented,wherein the structural regulation and electrochemical performance of the Mg-intercalation MnO_(2)(denoted as MMO)electrode were thoroughly investigated by density functional theory(DFT)calculations and in-situ Raman investigation.The results demonstrate that the Mg intercalation is essential to adjusting the charge/ion state and electronic band gap of MMO electrode,as well as the highly reversible phase transition of the MMO electrode during the charging-discharging process.Because of these remarkable characteristics,the MMO electrode can be capable of delivering a significant specific capacity of~419.8 mAh·g^(−1),while exhibiting a good cycling capability over 1000 cycles in 1 M aqueous MgCl_(2) electrolyte.On the basis of such MMO electrode,we have successfully developed a soft-packaging aqueous MIB with excellent electrochemical properties,revealing its huge application potential as the efficient energy storage devices.

The Influence of Alkaline Earth Elements on Electronic Properties ofα-Si3N4 via DFT Calculation

We used density functional theory(DFT)calculations to study the influence of alkali earth metal element(AE)doping on the crystal structure and electronic band structure ofα-Si3N4.The diversity of atomic radii of alkaline earth metal elements results in structural expansion when they were doped into theα-Si3N4 lattice.Formation energies of the doped structures indicate that dopants prefer to occupy the interstitial site under the nitrogen-deficient environment,while substitute Si under the nitrogen-rich environment,which provides a guide to synthesizingα-Si3N4 with different doping types by controlling nitrogen conditions.For electronic structures,energy levels of the dopants appear in the bottom of the conduction band or the top of the valence band or the forbidden band,which reduces the bandgap ofα-Si3N4.

New ordered MAX phase Mo_2 TiAlC_2: Elastic and electronic properties from first-principles

First-principles computation on the basis of density functional theory(DFT) is executed with the CASTEP code to explore the structural, elastic, and electronic properties along with Debye temperature and theoretical Vickers' hardness of newly discovered ordered MAX phase carbide Mo_2TiAlC_2. The computed structural parameters are very reasonable compared with the experimental results. The mechanical stability is verified by using the computed elastic constants. The brittleness of the compound is indicated by both the Poisson's and Pugh's ratios. The new MAX phase is capable of resisting the pressure and tension and also has the clear directional bonding between atoms. The compound shows significant elastic anisotropy. The Debye temperature estimated from elastic moduli(B, G) is found to be 413.6 K. The electronic structure indicates that the bonding nature of Mo_2TiAlC_2 is a mixture of covalent and metallic with few ionic characters. The electron charge density map shows a strong directional Mo–C–Mo covalent bonding associated with a relatively weak Ti–C bond.The calculated Fermi surface is due to the low-dispersive Mo 4d-like bands, which makes the compound a conductive one.The hardness of the compound is also evaluated and a high value of 9.01 GPa is an indication of its strong covalent bonding.

Tuning the photocatalytic water-splitting performance with the adjustment of diameter in an armchair WSSe nanotube

Due to the enigmatical electrostatic potential difference between the inside and outside layers,the relationship between the diameter and the photocatalytic property of the Janus transition metal dichalcogenides nanotube is still unclear.In this job,for the first time we calculate the electrostatic potential difference of the Janus WSSe armchair nanotubes with corresponding building block models through the first principles calculations.The electrostatic potential difference increases as the diameter increases.Then,it is observed that the WSSe armchair nanotubes with smaller diameter have stronger oxidation capacity,weaker reduction capacity,and higher solar-to-hydrogen conversion efficiency.Furthermore,the diminution of diameter could make the band gap drop,and even cause a direct-indirect transformation of band structure.The adjustment of diameter could also regulate the ability of adsorbing water molecules at the insider and outside layers.Moreover,the suitable band edge positions,wide optical absorbance region(to the near-infrared),outstanding solar-to-hydrogen efficiency(up to 28.99%),high carrier separation,adequate photoexcited carrier driving forces,as well as the energetic and thermal stability,render these nanotubes befitting the photocata lytic water-splitting application.Our study not only predicts a kind of ideal water-splitting photocatalyst,but also shows an effective way to improve their photocatalytic performances.

Zeolite-templated carbons as effective sorbents to remove methylsiloxanes and derivatives:A computational screening

Though widely used in our daily lives,volatile methylsiloxanes and derivatives are emerging contaminants and becoming a high-priority environment and public health concern.Developing effective sorbent materials can remove siloxanes in a cost-effective manner.Herein,by means of Grand Canonical Monte Carlo(GCMC)simulations,we evaluated the potentials of the recently proposed 68 stable zeolite-templated carbons(ZTCs)(PNAS 2018,115,E8116-E8124)for the removal of four linear methylsiloxanes and derivatives as well as two cyclic methylsiloxanes by the calculated average loading and average adsorption energy values.Four ZTCs,namely ISV,FAU1,FAU3,and H8326836,were identified with the top 50%adsorption performance toward all the six targeted contaminants,which outperform activated carbons.Further first principles computations revealed that steric hindrance,electrostatic interactions(further enhanced by charge transfer),and CH-p interactions account for the outstanding adsorption performance of these ZTCs.This work provides a quick procedure to computationally screen promising ZTCs for siloxane removal,and help guide future experimental and theoretical investigations.