Doping duo: Mesoporous graphene doped with both N and S atoms (N-S-G) was prepared in one step studied as an electrochemical catalyst for the oxygen reduction reaction (ORR). The shows excellent ORR performance comparable to that of commercial Pt/C. outstanding activity N-S-G results from large number synergistic effect dopant heteroatoms.

The electrocatalytic hydrogen-evolution reaction (HER), as the main step of water splitting and cornerstone exploring mechanism other multi-electron transfer electrochemical processes, is subject extensive studies. A large number high-performance electrocatalysts have been developed for HER accompanied by recent significant advances in its nature. Herein we present a critical appraisal both theoretical experimental studies with special emphasis on electronic structure, surface...

Organometallic complexes with metal–nitrogen/carbon (M–N/C) coordination are the most important alternatives to precious metal catalysts for oxygen reduction and evolution reactions (ORR OER) in energy conversion devices. Here, we designed developed a range of molecule-level graphitic carbon nitride (g-C3N4) coordinated transition metals (M–C3N4) as new generation M–N/C these electrode reactions. As proof-of-concept example, conducted theoretical evaluation experimental validation on...

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...

The mutually corroborated electrochemical measurements and density functional theory (DFT) calculations were used to uncover the origin of electrocatalytic activity graphene-based electrocatalysts for oxygen reduction reaction (ORR). A series graphenes doped with nonmetal elements was designed synthesized, their ORR performance evaluated in terms four descriptors: exchange current density, on-set potential, pathway selectivity kinetic density. It is shown that these descriptors are good...

Don't be a dope: double dope! Graphene was doped with both boron and nitrogen at well-defined doping sites to induce synergistic effect that boosts its catalytic activity for oxygen reduction (see structure). The excellent performance of the new metal-free catalyst is comparable commercial Pt/C. As service our authors readers, this journal provides supporting information supplied by authors. Such materials are peer reviewed may re-organized online delivery, but not copy-edited or typeset....

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%...

Replacement of precious Pt catalyst with cost-effective alternatives would be significantly beneficial for hydrogen production via electrocatalytic evolution reaction (HER). All candidates thus far are exclusively metallic catalysts, which suffer inherent corrosion and oxidation susceptibility during acidic proton-exchange membrane electrolysis. Herein, based on theoretical predictions, we designed synthesized nitrogen (N) phosphorus (P) dual-doped graphene as a nonmetallic electrocatalyst...

Hydrogen evolution reaction (HER) is a critical process due to its fundamental role in electrocatalysis. Practically, the development of high-performance electrocatalysts for HER alkaline media great importance conversion renewable energy hydrogen fuel via photoelectrochemical water splitting. However, both mechanistic exploration and materials under conditions are very limited. Precious Pt metal, which still serves as state-of-the-art catalyst HER, unable guarantee sustainable supply. Here...

Electrochemical reduction of CO2 to high-energy-density oxygenates and hydrocarbons beyond CO is important for long-term large-scale renewable energy storage. However, the key step C-C bond formation needed generation C2 products induces an additional barrier on reaction. This inevitably creates larger overpotentials greater variety as compared conversion C1 products. Therefore, in-depth understanding catalytic mechanism required advancing design efficient electrocatalysts control reaction...

The lack of chemical understanding and efficient catalysts impedes the development electrocatalytic nitrogen reduction reaction (eNRR) for ammonia production. In this work, we employed density functional theory calculations to build up a picture (activity trends, electronic origins, design strategies) single-atom (SACs) supported on nitrogen-doped carbons as eNRR electrocatalysts. To construct such picture, work presents systematic studies activity SACs covering 20 different transition metal...

Product selectivity in multielectron electrocatalytic reactions is crucial to energy conversion efficiency and chemical production. However, a present practical drawback the limited understanding of actual catalytic active sites. Here, using as prototype single-atom catalysts (SACs) acidic oxygen reduction reaction (ORR), we report structure–property relationship show for first time that molecular-level local structure, including second coordination spheres (CSs), rather than individual...

Abstract Engineering the surface structure at atomic level can be used to precisely and effectively manipulate reactivity durability of catalysts. Here we report tuning one-dimensional single-crystal cobalt (II) oxide (CoO) nanorods by creating oxygen vacancies on pyramidal nanofacets. These CoO exhibit superior catalytic activity towards reduction/evolution reactions. The combined experimental studies, microscopic spectroscopic characterization, density functional theory calculations reveal...

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....

Single-atom catalysts (SACs) have great potential in electrocatalysis. Their performance can be rationally optimized by tailoring the metal atoms, adjacent coordinative dopants, and loading. However, doing so is still a challenge because of limited synthesis approach insufficient understanding structure-property relationships. Herein, we report new kind Mo SAC with unique O,S coordination high loading over 10 wt %. The isolation local environment was identified high-angle annular dark-field...

A major impediment to the electrocatalytic CO2 reduction reaction (CRR) is lack of electrocatalysts with both high efficiency and good selectivity toward liquid fuels or other valuable chemicals. Effective strategies for design are yet be discovered substitute conventional trial-and-error approach. This work shows that a combination density functional theory (DFT) computation experimental validation molecular scaffolding coordinate metal active centers presents new molecular-level strategy...

Noble metals manifest themselves with unique electronic structures and irreplaceable activity toward a wide range of catalytic applications but are unfortunately restricted by limited choice geometric spanning single atoms, clusters, nanoparticles, bulk crystals. Herein, we propose how to overcome this limitation integrating noble metal atoms into the lattice transition oxides create new type hybrid structure. This study shows that iridium can be accommodated cationic sites cobalt spinel...

Designing high-performance and cost-effective electrocatalysts toward oxygen evolution hydrogen reactions in water-alkali electrolyzers is pivotal for large-scale sustainable production. Earth-abundant transition metal oxide-based catalysts are particularly active reaction; however, they generally considered inactive reaction. Here, we show that strain engineering of the outermost surface cobalt(II) oxide nanorods can turn them into efficient They competitive with best this reaction alkaline...