Qiang Sun

• PhD
• Professor (Full) at Peking University

Hydrogen fuel with zero CO2 emission is of current interest for global carbon neutralization. In this study, a 3D porous aluminum nitride (p‐AlN) framework assemble from AlN‐biphenylene nanoribbons and investigate its performance in reversible hydrogen storage is presented. Using density functional theory (DFT), it is showed that the p‐AlN is dynam...

In recent findings, a new classification of 1D and 2D tetrahexagonal boron nitrides (th-BN) consisting of square and hexagonal rings has been documented. These materials exhibit impressive properties such as the tunable band gap, strong optical absorption, suitable sign-tunable Poisson's ratio, and high ideal strength, making them promising for app...

To investigate the potential usage of sepiolite and palygorskite for subsurface hydrogen storage, the authors performed hydrogen adsorption measurements at different temperatures (25 °C, 45 °C and 65 °C) persisting constant atmospheric pressure and at different pressures (between 0 and 18 MPa) with a constant temperature (65 °C). Furthermore, hydro...

Motivated by the recent experimental synthesis of a LaCl3-based lithium superionic conductor [Yin, Y.-C. Nature 2023, 616, 77–83], we explore the potential of a LaCl3-based system for a sodium superionic conductor in this work. Using density functional theory combined with molecular dynamics simulation and a grand potential phase diagram analysis,...

Designing cage-based three-dimensional (3D) carbon allotropes is of significant interest due to their unique chemical and physical properties, along with fascinating applications in nanoelectronics, optoelectronics, and nanomechanics. Among the many studied carbon polymorphs, however, it is urgent to find 3D-ordered porous architectures with high h...

Motivated by the recent experimental study on hydrogen storage in MXene multilayers [Liu et al., Nat. Nanotechnol. 16, 331 (2021)], for the first time we propose a workflow to computationally screen 23 857 compounds of MXene to explore the general relation between the activated H2 bond length and adsorption distance. By using density functional the...

Na3V2(PO4)2F3 (NVPF) is a representative cathode material of sodium-ion batteries (SIBs) due to its high working voltage and high structural stability. However, its specific capacity is limited to the reversible inserting and extracting of two sodium ions per formula unit, which hampers the improvement of its energy density. In this study, we propo...

Tunning the micro-electric field at the metal-support interface offers great opportunities for developing heterogeneous catalysts with high stability, selectivity, and activity. However, the role of carbon support defects plays in manipulating the charge transfer process and activating the interfacial perimeter sites is still obscure due to the abs...

Motivated by the recent experimental study on hydrogen storage in MXene multilayers [Nature Nanotechnol. 2021, 16, 331], for the first time we propose a workflow to computationally screen 23,857 compounds of MXene to explore the general relation between the activated H2 bond length and adsorption distance. By using density functional theory (DFT),...

Inverse sandwich clusters composed of a monocyclic boron ring and two capping transition metal atoms are interesting alloy cluster systems, yet their chemical bonding nature has not been sufficiently elucidated to date. We report herein on the theoretical prediction of a new example of boron-based inverse sandwich alloy clusters, V2B7−, through com...

Designing novel crystalline materials composed of light and nontoxic elements, but with ultralow thermal conductivity insensitive to temperature, has been a long-standing challenge. One effective strategy is to utilize superatoms as building blocks to introduce hierarchical bonding and vibration for suppressing phonon velocity and enhancing high-or...

Disordered rock salt transition-metal oxides have emerged recently as promising electrodes for Li-ion batteries (LIBs). However, only two disordered rock salt (DRX) materials, Li3V2O5 and Li3Nb2O5, have been studied as anodes so far, leaving numerous DRX compounds with vast compositions and exotic battery-related performance unexplored. Here, based...

Doping alkali metals into boron clusters can effectively compensate for the intrinsic electron deficiency of boron and lead to interesting boron-based binary clusters, owing to the small electronegativity of the former elements. We report on the computational design of a three-layered sandwich cluster, Na5B7, on the basis of global-minimum (GM) sea...

Natural hydrogen has been widely detected in many environments. However, up to date, the knowledge about the occurrence of hydrogen in the geological formation is very limited. Clay minerals with large adsorption capacities due to their huge specific surface area are widely distributed in the subsurface. In order to find whether the hydrogen can be...

A plier-shaped charge-transfer [Mg 2 ] ²⁺ [Mg 2 B 7 ] ⁻ complex cluster exhibits double 6π/6σ aromaticity, whose hybrid molecular wheel structure is rationalized using the concept of electronic transmutation.

Superatomic materials are newly emerging candidates for high-performance thermoelectric (TE) devices due to their intrinsic ultralow thermal conductivities. However, the low TE power factor becomes a huge obstacle to reaching the required dimensionless figure of merit (ZT) values for practical applications. Here, motivated by the recently synthesiz...

Superatom-based superionic conductors are of current interest due to their promising applications in solid-state electrolytes for rechargeable batteries. However, much less attention has been paid to their thermal properties, which are vital for safety and performance. Motivated by the recent synthesis of superatom-based superionic conductor Na3OBH...

Scandate cathode as a thermionic electron emission material has attracted broad interest owing to its high electron emission capability. Despite the large number of studies on the electron emission of the scandate tungsten cathode, there is a lack of understanding of the performance of scandium oxide incorporated in other refractory metal matrix. I...

Extensive efforts are devoted to the design of new carbon materials with improved specific capacity for metal ion batteries (MIBs). One of the effective strategies for such material design is to change the structural unit. Recently, tetracene‐based nanoribbons have been synthesized (Chem. Eur. J. 2019, 25, 12074), which can be used as a basic build...

Na-ion batteries (NIBs) capture intensive research interest in large-scale energy storage applications because of sodium's abundant resources and low cost. However, the low capacity, poor conductivity, and short cycle life of the commonly used anodes are the main challenges in developing advanced NIBs. Here, stimulated by the recent successful synt...

Since the discovery of graphene, numerous efforts have been made to seek new two-dimensional (2D) graphenelike materials with intriguing properties. Here,we report a stable graphenelike supersalt NaNO3 monolayer composed of superhalogen NO3. The 2D NaNO3 monolayer is found to possess an ultralow isotropic Young's modulus (2.983 N/m) and a low therm...

Regulating surface strain of nanomaterials is an effective strategy to manipulate the activity of catalysts, yet not well recognized in the rechargeable Li‐CO2 batteries. Herein, biaxially compressive strained nickel/ruthenium core/shell hexagonal nanoplates (Ni/Ru HNPs) with lattice compression of ∼5.1% and ∼3.2% in the Ru {10‐10} and (0002) facet...

The 2019 Nobel Prize in Chemistry and the 2016 Nobel Prize in Physics were awarded for the research of lithium-ion batteries and topological quantum materials, respectively, which have greatly promoted the advances in these two fields. The high rate performance of a battery requires the anode to be conductive not just ionically but also electronica...

Although cyclobutene consisting of 4-membered rings of C atoms is highly unstable, one- and two-dimensional (1D, 2D) carbon allotropes, called tetrahexcarbon (th-C) consisting of 4- and 6- membered rings, have been reported recently, which shows novel properties with prominent applications in nano-electronics, optoelectronics, and nano-mechanics. G...

Fast charging electrode materials require excellent ion conductivity as well as high and stable electrical conductivity. However, the main commercial cathode materials are semiconducting transition metal oxides suffering from low electrical conductivity, so cathode materials with good electrical conductivity are highly desirable. It is well‐known t...

Utilizing molecular dynamics (MD) simulations based on the highly precise force-fields, we find that phonon scattering strengths induced by the cubic anharmonicity can be significantly underestimated by the perturbation theory (PT) approach in materials with sizable frequency gaps or branch bunching. We trace this result to the additional three-pho...

Conversion of waste heat into usable energy requires development of thermoelectric materials with high efficiency in a wide temperature range. Using first principles theory and Boltzmann transport theory, we show that the thermoelectric performance of the p-type single-layer Sb2Si2Te6 has a high figure of merit ZT of 2.62 at 900 K and a record high...

Nearly half a century of research on atomic clusters has revealed many exciting and unexpected properties of this new phase of matter. This book summarizes the recent developments in the rational design of superatoms using different electron‐counting rules, applied individually or in combination. One‐, two‐, and three‐dimensional cluster‐based mate...

Since the discovery of graphene, 2D carbon materials and their assembled 3D porous materials have been hotly pursued. Motivated by the recent successful synthesis of biphenylene [Science 372 (2021) 852], we design a biphenylene-nanoribbon-based 3D porous carbon allotrope. The assembled structure (named Tet-C52) possesses excellent stability, low ma...

Cluster-assembled materials are expected to possess properties very different from those where individual atoms form the building blocks. A case in point is fullerite composed of C 60 fullerenes. Because of its size, symmetry, and intrinsic bonding features, properties of fullerite are different from graphite or diamond that are built from individu...

Development of efficient thermoelectric materials that convert waste heat into useable energy is important in addressing the impending energy and environmental crisis. In this chapter, we discuss how materials based on clusters as building blocks can be useful in the design and synthesis of a new class of materials with reduced lattice thermal cond...

This chapter deals with the rational design of superatomic clusters that mimic the chemistry of atoms using electron-counting rules, some of which have been in use for more than a century. These rules include the jellium rule for clusters composed of free-electron metals, octet rule for low atomic number elements, 18-electron rule for transition me...

Carbon dioxide (CO 2 ) is a greenhouse gas that is primarily responsible for global warming. Consequently, there is considerable interest in studying the capture, sequestration, and conversion of CO 2 . Catalysts play an important role in this regard. In this chapter we review some of the recent developments in the role of clusters in CO 2 activati...

Hafnium (Hf) has been used as a cathode material for thermionic emission in high temperature environments for a long time. However, the effect of grain boundaries (GBs) on its work function has not been reported. In this work, by using first-principles calculations, we find that the introduction of GBs would reduce the work function of Hf surface a...

It is well established that metal atoms can be used to regulate porosity in synthesis and porous structures can be obtained by removing metal atoms. Motivated by a recent synthesis of 2Sr@B6C6, it is found that when Sr atoms are removed, the resulting 3D porous BC structure (3D‐B6C6) with reduced symmetry is stable thermally, dynamically, and mecha...

The development of renewable and clean energy technologies requires the design of efficient materials for a wide variety of electrochemical applications. Using density functional theory, we design two metallic borophene-based three-dimensional (3D) porous structures (termed 3D-β 12-borophene and 3D-B 7 P 2), which are found to be dynamically, therm...

Halide materials are of current interest for all-solid-state batteries. In this study, we systematically studied seven fluorides Li3MF6 (M = Al, Sc, Ti, V, Cr, Ga, In) using density functional theory combined with molecular dynamics simulation and the grand potential phase diagram analysis. Among them, Li3ScF6 is identified to be a promising solid...

The high rate performance of a battery requires the anode to be conductive not just ionically but also electronically. This criterion has significantly stimulated the study on 3D porous topological metals composed of nonmetal atoms with a light mass. Many carbon-based 3D topological metals for batteries have been reported, while similar work for 3D...

Metallic materials composed of light and rich abundant element like carbon is of current interest in battery technology. In this study, according to the features of 3D pentadiamond reported recently, we propose a two-dimensional (2D) pentadiamond monolayer C558 composed of pentagons and octagons. Based on first-principles calculations we show that...

Materials composed of B, C, and P have been hotly pursued for batteries due to their light mass and rich abundance. However, all the reported 3D B-C-P compounds at present are semiconductors with low electric conductivity. Motivated by the semi-metallic character of a stable 2D-BPC2 sheet, we propose the first metallic porous 3D structure by using...

Li metal batteries have attracted extensive research attention because of their extremely high theoretical capacity. However, the commercialization of the Li metal batteries is hindered, as uncontrolled Li dendrites growth leads to safety concerns and a low coulombic efficiency. To suppress Li dendrites growth and achieve dense Li deposition, a lit...

Motivated by the recent synthesis of three-dimensional (3D) porous borocarbonitride (Angew. Chem. Int. Ed. 2019, 58, 6033), we propose a porous 3D-BC2N structure composed of BC2N nanoribbons. On the basis of detailed theoretical analysis and calculations, we find that the porous 3D-BC2N is dynamically stable with cohesive energy of 9.52 eV/atom and...

The front cover artwork is provided by the group of Prof. Qiang Sun (Peking University, China). The image shows how Cu‐decorated zigzag graphene nanoribbons can catalyze CO2 reduction to ethanol with a small energy barrier and tunable selectivity. Read the full text of the Article at 10.1002/cphc.202000476.

Development of anode materials is critical to the success of sodium ion batteries (SIBs). Because of the size difference between Li and Na, the commercial anode material graphite in Li-ion battery does not work for Na-ion battery. Thus, it will be ideal if some universal anode materials could work for both Li- and Na-ion batteries with high perform...

The Front Cover shows how a Cu‐decorated zigzag graphene nanoribbon is capable of catalyzing CO2 reduction to ethanol with a small energy barrier and tunable selectivity. More information can be found in the Article by Haoming Shen and Qiang Sun.

Nano-sheets Al2O3 supported CeO2-Fe2O3 binary oxides were prepared by the vacuum impregnation method. The structural and textural properties were characterized by pertinent techniques, and the materials were evaluated as catalysts for the oxidative dehydrogenation of ethylbenzene with carbon dioxide (CO2-ODEB). The characterization results show tha...

Cu catalysts are well‐known for their good performance in CO2 conversion. Compared to CO and CH4 production, C2 products have higher volumetric energy densities and are more valuable in industrial applications. In this work, we screened the catalytic ability of C2 production on several 1D Cu atomic chain structures and find that Cu edge‐decorated z...

The unique electronic configuration endows carbon with super-flexible bonding ability, displaying metallic, semi-conducting and insulating features with unprecedented applications. Inspired by the pressure–temperature phase diagram that clearly shows the phases (solid/liquid/gas) of a substance in different conditions, for the first time, we have d...

Lithium–sulfur batteries are promising energy‐storage devices because of their high theoretical energy densities. For practical Li–S batteries, reducing the amount of electrolyte used is essential for achieving the high energy densities. However, reducing the electrolyte amount leads to severe performance degradation, mainly because of sluggish dep...

An ideal electrode for electrochemical storage of hydrogen needs to be conductive for electron. The robust conductivity protected by topology in topological quantum materials just meets this requirement. However, such study is still lacking so far. Herein, for the first time, we explore the performance of hydrogen storage in topological quantum mat...

Carbon nanomaterials show the potential in achieving the potassium ion storage, however, the limited interlayer spacing in the existed carbon nanomaterials greatly impact the performance of PIBs. Herein, we report a class of 3D porous carbon framework material constructed by S/N co-doping graphene nanosheets (CFM-SNG) with ultra-large interlayer sp...

Boron-based 2D materials are of current interest. However, graphene-like geometry is unstable for B due to the electron deficiency, which can be stabilized by introducing H, F and Cl. Here, using density functional theory combined with phonon Boltzmann transport equation, we perform systematic studies on how the functionalization changes the lattic...

All-solid-state sodium-ion batteries (ASIBs) are promising candidates for large-scale energy storage applications. To build such a battery system, efficient solid-state electrolytes (SSEs) with high sodium ionic conductivity at room temperature and good electrochemical stability as well as interface compatibility are required. In this work, using d...

Considering the problems of high costs, low catalytic activity and selectivity in the metal‐based catalysts for CO2 electroreduction, we apply boron‐containing metal‐free B2S sheet as an alternative to the traditional metal‐based catalysts. Reaction energy calculations identify the preferred “Formate” pathway for CO2 conversion to CH3OH on B2S, in...

High energy density, low cost, and environmental friendliness are required for modern energy‐storage technologies. The anchoring performance of newly fabricated porous triphenylene–graphdiyne (TPGDY), boron–graphdiyne (BGDY), and nitrogen–graphdiyne (NDGY–C18N6, NGDY–C24N4, and NGDY–C36N6) monolayers are studied by employing density functional theo...

The ferromagnetism in Cr-trihalide monolayers is of current interest [Nat. Nanotech. 2019,14, 408], however, its Currie temperature is low. How can we enhance the thermal stability of ferromagnetism? Motivated by the recent synthesis of the layered conductive magnet CrCl2(pyrazine)2 [Nat. Chem. 2018, 10, 1056], we perform first-principles calculati...

Cu catalysts are well-known for their good performance in CO2 conversion, and Cu atomic catalysts supported porous 2D materials are of special interest for CO2 electroreduction. In this work, we have explored the catalytic properties of Cu atomic catalysts supported on the newly synthesized triphenylene-graphdiyne [ACS Appl. Mater. Interfaces 2019,...

Motivated by the recent synthesis of two-dimensional (2D) metal–organic frameworks TM3(HAB)2 (TM = Fe, Co, Ni, Cu; HAB = hexaaminobenzene) with good intrinsic conductivity, for the first time we explore the CO2 conversion performance of these 2D sheets using density functional theory combined with computational hydrogen electrode model. We find Fe3...

Due to the compatibility with the well-developed Si-based semiconductor technology, the properties of silicene and silicene-based materials have attracted tremendous attention. Among them, the thermal conductivity (TC) is of special importance for electronic devices. However, unlike graphene, the poor quality of empirical potentials hinders the rel...

The structural stabilities and electronic properties are studied for the recently synthesized one‐dimensional (1‐D) tetracene‐based nanoribbons with four‐membered rings by using first‐principles calculation. All three configurations (named as straight, zigzag, and armchair) are stable and exhibit an indirect band gap of 1.46, 0.73, and 0.32 eV, res...

CuS micro-flowers self-assembled by nanosheets were prepared by hydrothermal synthesis (HS) using CuCl2·2H2O and CS(NH2)2 as raw materials, glycol as a solvent at 120 and 140 ℃ for 1.5 h. With increasing hydrothermal temperature or reaction time, the CuS micro-flowers break up to Cu1.8S nanoparticles. The single phase Cu1.8S nanoparticles were obta...

Search for novel cathode materials is of current interest. Among them, Li2MnSiO4 shows promise as a cathode material in the poly-anion family due to its structural diversity, abundance, low cost, and high theoretical capacity (330 mAh/g). However, it suffers from low electronic and ionic conductivity, limited reversible capacity, and poor cycling p...

Bismuth compounds have been playing an important role in thermoelectric (TE) applications. To match the high figure of merit (ZT) of n-type Bi-based TE materials for constructing effective TE devices, searching for p-type Bi-based TE materials with high ZT is highly desirable. Inspired by the successful exfoliation of BiOBr atomic layers [Wu et al....

Motivated by the advantages of inherent high electronic conductivity and ordered porosity of topological semimetal monoclinic C16 (m-C16), we explore its possibility for lithium-ion battery anode material. Using state-of-the-art theoretical calculations, we show that m-C16 structure has a high specific capacity of 558 mAh/g, low Li ion diffusion en...