Three parallel algorithms for classical molecular dynamics are presented. The first assigns each processor a fixed subset of atoms; the second assigns each a fixed subset of inter-atomic forces to compute; the third assigns each a fixed spatial region. The algorithms are suitable for molecular dynamics models which can be difficult to parallelize efficiently—those with short-range forces where the neighbors of each atom change rapidly. They can be implemented on any distributed-memory parallel machine which allows for message-passing of data between independently executing processors. The algorithms are tested on a standard Lennard-Jones benchmark problem for system sizes ranging from 500 to 100,000,000 atoms on several parallel supercomputers--the nCUBE 2, Intel iPSC/860 and Paragon, and Cray T3D. Comparing the results to the fastest reported vectorized Cray Y-MP and C90 algorithm shows that the current generation of parallel machines is competitive with conventional vector supercomputers even for small problems. For large problems, the spatial algorithm achieves parallel efficiencies of 90% and a 1840-node Intel Paragon performs up to 165 faster than a single Cray C9O processor. Trade-offs between the three algorithms and guidelines for adapting them to more complex molecular dynamics simulations are also discussed.

Fast parallel algorithms for short-range molecular dynamics

Intermolecular And Surface Forces

As one important component of sulfur cathodes, the carbon host plays a key role in the electrochemical performance of lithium-sulfur (Li-S) batteries. In this paper, a mesoporous nitrogen-doped carbon (MPNC)-sulfur nanocomposite is reported as a novel cathode for advanced Li-S batteries. The nitrogen doping in the MPNC material can effectively promote chemical adsorption between sulfur atoms and oxygen functional groups on the carbon, as verifi ed by X-ray absorption near edge structure spectroscopy, and the mechanism by which nitrogen enables the behavior is further revealed by density functional theory calculations. Based on the advantages of the porous structure and nitrogen doping, the MPNC-sulfur cathodes show excellent cycling stability (95% retention within 100 cycles) at a high current density of 0.7 mAh cm −2 with a high sulfur loading (4.2 mg S cm −2 ) and a sulfur content (70 wt%). A high areal capacity (≈3.3 mAh cm −2 ) is demonstrated by using the novel cathode, which is crucial for the practical application of Li-S batteries. It is believed that the important role of nitrogen doping promoted chemical adsorption can be extended for development of other high performance carbon-sulfur composite cathodes for Li-S batteries.

Nitrogen-Doped Mesoporous Carbon Promoted Chemical Adsorption of Sulfur and Fabrication of High-Areal-Capacity Sulfur Cathode with Exceptional Cycling Stability for Lithium-Sulfur Batteries

Catalytic transformations of syngas (a mixture of H2 and CO), which is one of the most important C1-chemistry platforms, and CO2, a greenhouse gas released from human industrial activities but also a candidate of abundant carbon feedstock, into chemicals and fuels have attracted much attention in recent years. Fischer-Tropsch (FT) synthesis is a classic route of syngas chemistry, but the product selectivity of FT synthesis is limited by the Anderson-Schulz-Flory (ASF) distribution. The hydrogenation of CO2 into C2+ hydrocarbons involving C-C bond formation encounters similar selectivity limitation. The present article focuses on recent advances in breaking the selectivity limitation by using a reaction coupling strategy for hydrogenation of both CO and CO2 into C2+ hydrocarbons, which include key building-block chemicals, such as lower (C2-C4) olefins and aromatics, and liquid fuels, such as gasoline (C5-C11 hydrocarbons), jet fuel (C8-C16 hydrocarbons) and diesel fuel (C10-C20 hydrocarbons). The design and development of novel bifunctional or multifunctional catalysts, which are composed of metal, metal carbide or metal oxide nanoparticles and zeolites, for hydrogenation of CO and CO2 to C2+ hydrocarbons beyond FT synthesis will be reviewed. The key factors in controlling catalytic performances, such as the catalyst component, the acidity and mesoporosity of the zeolite and the proximity between the metal/metal carbide/metal oxide and zeolite, will be analysed to provide insights for designing efficient bifunctional or multifunctional catalysts. The reaction mechanism, in particular the activation of CO and CO2, the reaction pathway and the reaction intermediate, will be discussed to provide a deep understanding of the chemistry of the new C1 chemistry routes beyond FT synthesis.

New horizon in C1 chemistry: breaking the selectivity limitation in transformation of syngas and hydrogenation of CO2 into hydrocarbon chemicals and fuels

Water electrolysis represents a promising sustainable hydrogen production technology. However, in practical application which requires extremely large current densities (>500 mA cm−2), the oxygen evolution reaction (OER) becomes unstable and kinetically sluggish, which is a major hurdle to large-scale hydrogen production. Herein, we report an exceptionally active and binder-free NiFe nanowire array based OER electrode that allows durable water splitting at current densities up to 1000 mA cm−2 up to 120 hours. Specifically, NiFe oxyhydroxide (shell)–anchored NiFe alloy nanowire (core) arrays are prepared via a magnetic-field-assisted chemical deposition method. The ultrathin (1–5 nm) and amorphous NiFe oxyhydroxide is in situ formed on the NiFe alloy nanowire surface, which is identified as an intrinsically highly active phase for the OER. Additionally, the fine geometry of the hierarchical electrode can substantially improve charge and mass (reactants and oxygen bubbles) transfer. In an alkaline electrolyte, this OER electrode can yield current densities of 500 and 1000 mA cm−2 stably over 120 hours at overpotentials of only 248 mV and 258 mV respectively, which are dramatically lower than any recently reported overpotentials. Notably, the integrated alkaline electrolyzer (with pure Ni nanowires as HER electrode) is demonstrated to reach the current density of 1000 mA cm−2 with super low voltage of 1.76 V, outperforming the state-of-the-art industrial catalysts. Our result may represent a critical step towards an industrial electrolyzer for large-scale hydrogen production by water splitting.

Exceptional performance of hierarchical Ni–Fe oxyhydroxide@NiFe alloy nanowire array electrocatalysts for large current density water splitting

High-entropy alloys are a class of materials that contain five or more elements in near-equiatomic proportions1,2. Their unconventional compositions and chemical structures hold promise for achieving unprecedented combinations of mechanical properties3–8. Rational design of such alloys hinges on an understanding of the composition–structure–property relationships in a near-infinite compositional space9,10. Here we use atomic-resolution chemical mapping to reveal the element distribution of the widely studied face-centred cubic CrMnFeCoNi Cantor alloy2 and of a new face-centred cubic alloy, CrFeCoNiPd. In the Cantor alloy, the distribution of the five constituent elements is relatively random and uniform. By contrast, in the CrFeCoNiPd alloy, in which the palladium atoms have a markedly different atomic size and electronegativity from the other elements, the homogeneity decreases considerably; all five elements tend to show greater aggregation, with a wavelength of incipient concentration waves11,12 as small as 1 to 3 nanometres. The resulting nanoscale alternating tensile and compressive strain fields lead to considerable resistance to dislocation glide. In situ transmission electron microscopy during straining experiments reveals massive dislocation cross-slip from the early stage of plastic deformation, resulting in strong dislocation interactions between multiple slip systems. These deformation mechanisms in the CrFeCoNiPd alloy, which differ markedly from those in the Cantor alloy and other face-centred cubic high-entropy alloys, are promoted by pronounced fluctuations in composition and an increase in stacking-fault energy, leading to higher yield strength without compromising strain hardening and tensile ductility. Mapping atomic-scale element distributions opens opportunities for understanding chemical structures and thus providing a basis for tuning composition and atomic configurations to obtain outstanding mechanical properties. In high-entropy alloys, atomic-resolution chemical mapping shows that swapping some of the atoms for larger, more electronegative elements results in atomic-scale modulations that produce higher yield strength, excellent strain hardening and ductility.

Tuning element distribution, structure and properties by composition in high-entropy alloys.

Conductive and Catalytic Triple-Phase Interfaces Enabling Uniform Nucleation in High-Rate Lithium–Sulfur Batteries

Single-atom catalysts (SACs) have great potential in electrocatalysis. Their performance can be rationally optimized by tailoring the metal atoms, adjacent coordinative dopants, and metal loading. However, doing so is still a great challenge because of the limited synthesis approach and insufficient understanding of the structure-property relationships. Herein, we report a new kind of Mo SAC with a unique O,S coordination and a high metal loading over 10 wt %. The isolation and local environment was identified by high-angle annular dark-field scanning transmission electron microscopy and extended X-ray absorption fine structure. The SACs catalyze the oxygen reduction reaction (ORR) via a 2 e- pathway with a high H2 O2 selectivity of over 95 % in 0.10 m KOH. The critical role of the Mo single atoms and the coordination structure was revealed by both electrochemical tests and theoretical calculations.

Coordination Tunes Selectivity: Two-Electron Oxygen Reduction on High-Loading Molybdenum Single-Atom Catalysts

Surface reactions constitute the foundation of various energy conversion/storage technologies, such as the lithium-sulfur (Li-S) batteries. To expedite surface reactions for high-rate battery applications demands in-depth understanding of reaction kinetics and rational catalyst design. Now an in situ extrinsic-metal etching strategy is used to activate an inert monometal nitride of hexagonal Ni3 N through iron-incorporated cubic Ni3 FeN. In situ etched Ni3 FeN regulates polysulfide-involving surface reactions at high rates. Electron microscopy was used to unveil the mechanism of in situ catalyst transformation. The Li-S batteries modified with Ni3 FeN exhibited superb rate capability, remarkable cycling stability at a high sulfur loading of 4.8 mg cm-2 , and lean-electrolyte operability. This work opens up the exploration of multimetallic alloys and compounds as kinetic regulators for high-rate Li-S batteries and also elucidates catalytic surface reactions and the role of defect chemistry.

Activating Inert Metallic Compounds for High-Rate Lithium-Sulfur Batteries Through In Situ Etching of Extrinsic Metal.

Lithium-sulfur (Li-S) batteries hold great promise to serve as next-generation energy storage devices. However, the practical performances of Li-S batteries are severely limited by the sulfur cathode regarding its low conductivity, huge volume change, and the polysulfide shuttle effect. The first two issues have been well addressed by introducing mesoporous carbon hosts to the sulfur cathode. Unfortunately, the nonpolar nature of carbon materials renders poor affinity to polar polysulfides, leaving the shuttling issue unaddressed. In this contribution, atomic cobalt is implanted within the skeleton of mesoporous carbon via a supramolecular self-templating strategy, which simultaneously improves the interaction with polysulfides and maintains the mesoporous structure. Moreover, the atomic cobalt dopants serve as active sites to improve the kinetics of the sulfur redox reactions. With the atomic-cobalt-decorated mesoporous carbon host, a high capacity of 1130 mAh gS-1 at 0.5 C and a high stability with a retention of 74.1% after 300 cycles are realized. Implanting atomic metal in mesoporous carbon demonstrates a feasible strategy to endow nanomaterials with targeted functions for Li-S batteries and broad applications.

Xiao Chen

Papers

Tuning element distribution, structure and properties by composition in high-entropy alloys.

Conductive and Catalytic Triple-Phase Interfaces Enabling Uniform Nucleation in High-Rate Lithium–Sulfur Batteries

Coordination Tunes Selectivity: Two-Electron Oxygen Reduction on High-Loading Molybdenum Single-Atom Catalysts

Activating Inert Metallic Compounds for High-Rate Lithium-Sulfur Batteries Through In Situ Etching of Extrinsic Metal.

Implanting Atomic Cobalt within Mesoporous Carbon toward Highly Stable Lithium–Sulfur Batteries