Abstract Scalable and sustainable solar hydrogen production through photocatalytic water splitting requires highly active stable earth-abundant co-catalysts to replace expensive rare platinum. Here we employ density functional theory calculations direct atomic-level exploration, design fabrication of a MXene material, Ti 3 C 2 nanoparticles, as efficient co-catalyst. nanoparticles are rationally integrated with cadmium sulfide via hydrothermal strategy induce super high visible-light...

Reducing carbon dioxide to hydrocarbon fuel with solar energy is significant for high-density storage and balance. In this work, single atoms of palladium platinum supported on graphitic nitride (g-C3N4), i.e., Pd/g-C3N4 Pt/g-C3N4, respectively, acting as photocatalysts CO2 reduction were investigated by density functional theory calculations the first time. During reduction, individual metal function active sites, while g-C3N4 provides source hydrogen (H*) from evolution reaction. The...

Defects derived by the removal of heteroatoms from graphene are demonstrated, both experimentally and theoretically, to be effective for all three basic electrochemical reactions, e.g., oxygen reduction (ORR), evolution (OER), hydrogen (HER). Density function theory calculations further reveal that different types defects essential individual electrocatalytic activity ORR, OER, HER, respectively.

Based on theoretical prediction, a g-C3N4@carbon metal-free oxygen reduction reaction (ORR) electrocatalyst was designed and synthesized by uniform incorporation of g-C3N4 into mesoporous carbon to enhance the electron transfer efficiency g-C3N4. The resulting composite exhibited competitive catalytic activity (11.3 mA cm–2 kinetic-limiting current density at −0.6 V) superior methanol tolerance compared commercial Pt/C catalyst. Furthermore, it demonstrated significantly higher (nearly 100%...

Developing highly conductive, stable, and active nonprecious hydrogen evolution reaction (HER) catalysts is a key step for the proposed economy. However, few catalysts, except noble metals, meet all requirements. By using state-of-the-art density functional calculations, herein we demonstrate that 2D MXenes, like Ti2C, V2C, Ti3C2, are terminated by mixture of oxygen atoms hydroxyl, while Nb2C Nb4C3O2 fully under standard conditions [pH 0, p(H2) = 1 bar, U 0 V vs electrode], findings in good...

Herein, the authors demonstrate a heterostructured NiFe LDH-NS@DG10 hybrid catalyst by coupling of exfoliated Ni-Fe layered double hydroxide (LDH) nanosheet (NS) and defective graphene (DG). The has exhibited extremely high electrocatalytic activity for oxygen evolution reaction (OER) in an alkaline solution with overpotential 0.21 V at current density 10 mA cm-2 , which is comparable to record (≈0.20 Fe-Co-Ni metal-oxide-film system) superior all other non-noble metal catalysts. Also, it...

Solar nitrogen (N2) fixation is the most attractive way for sustainable production of ammonia (NH3), but development a highly active, long-term stable and low-cost catalyst remains great challenge. Current research efforts N2 reduction mainly focus on metal-based catalysts using electrochemical approach, while metal-free or solar-driven have been rarely explored. Herein, basis concept electron "acceptance-donation", photocatalyst, namely, boron (B) atom, decorated optically active...

Opening up a band gap and finding suitable substrate material are two big challenges for building graphene-based nanodevices. Using state-of-the-art hybrid density functional theory incorporating long-range dispersion corrections, we investigate the interface between optically active graphitic carbon nitride (g-C3N4) electronically graphene. We find an inhomogeneous planar promotes electron-rich hole-rich regions, i.e., forming well-defined electron–hole puddle, on supported graphene layer....

Lead (Pb) free non-toxic perovskite solar cells have become more important in the commercialization of photovoltaic devices. In this study structural, electronic, optical and mechanical properties Pb-free inorganic metal halide cubic perovskites CsBX3 (B = Sn, Ge; X I, Br, Cl) for are simulated using first-principles Density Functional Theory (DFT). These compounds semiconductors with direct band gap energy mechanically stable. Results suggest that materials high absorption coefficient, low...

Solution-phase photocatalytic reduction of graphene oxide to reduced (RGO) by titanium dioxide (TiO2) nanoparticles produces an RGO-TiO2 composite that possesses enhanced charge transport properties beyond those pure TiO2 nanoparticle films. These films exhibit electron lifetimes up four times longer than intrinsic due RGO acting as a highly conducting intraparticle network within the film. The UV-active generation (photocurrent) was factor 10 incorporating RGO; we attribute this both...

Inspired by recent experiments on the successful fabrication of monolayer Janus transition-metal dichalcogenides [Lu, A.-Y.; Nat. Nanotechnol. 2017, 12, (8), 744 and ferromagnetic VSe2 [Bonilla, M.; 2018, 13, (4), 289], we predict a highly stable room-temperature (VSSe) density functional theory methods further confirmed stability global minimum search with particle-swarm optimization method. The VSSe exhibits large valley polarization due to broken space- time-reversal symmetry. Moreover,...

Abstract Electrocatalytic or photocatalytic N 2 reduction holds great promise for green and sustainable NH 3 production under ambient conditions, where an efficient catalyst plays a crucial role but remains long‐standing challenge. Here, high‐throughput screening of catalysts among (nitrogen‐doped) graphene‐supported single atom is performed based on general two‐step strategy. 10 promising candidates with excellent performance are extracted from 540 systems. Most strikingly, W embedded in...

We theoretically extend the applications of graphdiyne, an experimentally available one-atom-thin carbon allotrope, to nanoelectronics and superior separation membrane for hydrogen purification on a precise level.

Oxygen vacancy (VO ) engineering is an effective method to tune the photoelectrochemical (PEC) performance, but influence of VO on photoelectrodes not well understood. Using hematite as a prototype, we herein report that functions in more complicated way PEC process than previously reported. Through comprehensive analysis key charge transfer and surface reaction steps processes photoanode, clarify can facilitate electrocatalytic while leading severe interfacial recombination at...

The phase transition of single layer molybdenum disulfide (MoS2) from semiconducting 2H to metallic 1T and then 1T′ phases, the effect on hydrogen evolution reaction (HER) are investigated within this work by density functional theory. Experimentally, 2H-MoS2 has been widely used as an excellent electrode for HER can get charged easily. Here we find that negative charge a significant impact structural in MoS2 monolayer. thermodynamic stability 1T-MoS2 increases with state, comparing...

The lack of an obvious "band gap" is a formidable hurdle for making nanotransistor from graphene. Here, we use density functional calculations to demonstrate the first time that porosity such as evidenced in recently synthesized porous graphene (http://www.sciencedaily.com/releases/2009/11/091120084337.htm) opens band gap. size gap (3.2 eV) comparable most popular photocatalytic titania and graphitic C3N4 materials. In addition, adsorption hydrogen on Li-decorated much stronger than regular...

Increasing concerns about the atmospheric CO2 concentration and its impact on environment are motivating researchers to discover new materials technologies for efficient capture conversion. Here, we report a study of adsorption CO2, CH4, H2 boron nitride (BN) nanosheets nanotubes (NTs) with different charge states. The results show that process capture/release can be simply controlled by switching on/off charges carried BN nanomaterials. molecules form weak interactions uncharged...

Despite a suitable bandgap of bismuth vanadate (BiVO4 ) for visible light absorption, most the photogenerated holes in BiVO4 photoanodes are vanished before reaching surfaces oxygen evolution reaction due to poor charge separation efficiency bulk. Herein, new sulfur oxidation strategy is developed prepare planar with situ formed vacancies, which increases majority carrier density and photovoltage, leading record 98.2% among reported photoanodes. Upon loading NiFeOx as an cocatalyst, stable...

Abstract Owing to the sluggish kinetics for water oxidation, severe surface charge recombination is a major energy loss that hinders efficient photoelectrochemical (PEC) splitting. Herein, simple process developed preparing new type of low‐cost iron‐cobalt oxide (FeCoO x ) as an co‐catalyst suppress on bismuth vanadate (BiVO 4 photoanodes. The FeCoO /BiVO photoanode exhibits high photocurrent density 4.82 mA cm −2 at 1.23 V versus reversible hydrogen electrode under AM 1.5 G illumination,...

Transition metal-free magnetism and half-metallicity recently has been the subject of intense research activity due to its potential in spintronics application. Here we, for first time, demonstrate via density functional theory that most experimentally realized graphitic carbon nitride (g-C4N3) displays a ferromagnetic ground state. Furthermore, this novel material is predicted possess an intrinsic never reported date. Our results highlight new promising toward realistic

Atomic co-catalysts offer high potential to improve the photocatalytic performance, of which preparation with earth-abundant elements is challenging. Here, a new molten salt method (MSM) designed prepare atomic Ni co-catalyst on widely studied TiO2 nanoparticles. The liquid environment and space confinement effect leads dispersion ions TiO2, while strong polarizing force provided by promotes formation Ni−O bonds. Interestingly, atoms are found facilitate oxygen vacancies (OV) during MSM...

Abstract Controllably constructing nitrogen‐modified divacancies (ND) in carbon substrates to immobilize atomic Fe species and unveiling the advantageous configuration is still challenging, but indispensable for attaining optimal Fe−N−C catalysts oxygen reduction reaction (ORR). Herein, a fundamental investigation of unfolding intrinsically superior edge‐ND trapped motifs (e‐ND−Fe) relative an intact center model (c‐ND−Fe) ORR electrocatalysis reported. Density functional theory calculations...