Seawater electrolysis is an ideal approach to generating green hydrogen. Nevertheless, the sluggish kinetics of water dissociation and the detrimental chlorine chemistry environment are serious obstructions for industrial applications. Herein, constructing unique (Co) Lewis acid and (Ru-P) base pair sites in Ru-CoP decorated on nitrogen and phosphorus co-doped carbon (Ru-CoP/NPC) significantly optimizes the energy barrier of water dissociation and enhances the anti-corrosive ability for alkaline seawater splitting.
View Article and Find Full Text PDFDeveloping highly active and durable air cathode catalysts is crucial yet challenging for rechargeable zinc-air batteries. Herein, a size-adjustable, flexible, and self-standing carbon membrane catalyst encapsulating adjacent Cu/Na dual-atom sites is prepared using a solution blow spinning technique combined with a pyrolysis strategy. The intrinsic activity of the Cu-N site is boosted by the neighboring Na-containing functional group, which enhances O adsorption and optimizes the rate-determining step of O activation (*O → *OOH) during the oxygen reduction reaction process.
View Article and Find Full Text PDFElectrochemical seawater splitting is an intriguing strategy for green hydrogen production. Constructing advanced electrocatalysts for the hydrogen evolution reaction (HER) in seawater is extremely demanded for accelerating the sluggish kinetic process. Herein, a Ru nanocluster anchored on boron- and nitrogen-doped carbon (Ru/NBC) catalyst was successfully synthesized for the HER in alkaline/seawater electrolytes.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2023
Introducing a second metal species into atomically dispersed metal-nitrogen-carbon (M-N-C) catalysts to construct diatomic sites (DASs) is an effective strategy to elevate their activities and stabilities. However, the common pyrolysis-based method usually leads to substantial uncertainty for the formation of DASs, and the precise identification of the resulting DASs is also rather difficult. In this regard, we developed a two-step specific-adsorption strategy (pyrolysis-free) and constructed a DAS catalyst featuring FeCo "molecular heterostructures" (FeCo-MHs).
View Article and Find Full Text PDFSingle-atom catalysts (SACs) have attracted wide attention to be acted as potential electrocatalysts for nitrogen reduction reaction (NRR). However, the coordination environment of the single transition metal (TM) atoms is essential to the catalytic activity for NRR. Herein, we proposed four types of 3-, 4-coordinated and π-d conjugated TM B N S (x=2, 3, TM=Ti, V, Cr, Mn, Fe, Zr, Nb, Mo, Tc, Ru, Hf, Ta, W, Re and Os) monolayers for SACs.
View Article and Find Full Text PDFElectrocatalytic hydrogen evolution reaction (HER) is a promising way to produce pure and clean hydrogen. However, the preparation of efficient and economical catalysts for pH-universal HER remains a challenging but rewarding task. Herein, ultrathin RuZn nanosheets (NSs) with moiré superlattices and abundant edges are synthesized.
View Article and Find Full Text PDFHigh stability and efficiency of electrocatalysts are crucial for hydrogen evolution reaction (HER) toward water splitting in an alkaline media. Herein, a novel nano-Pt/Nb-doped Co(OH) (Pt/NbCo(OH) ) nanosheet is designed and synthesized using water-bath treatment and solvothermal reduction approaches. With nano-Pt uniformly anchored onto NbCo(OH) nanosheet, the synthesized Pt/NbCo(OH) shows outstanding electrocatalytic performances for alkaline HER, achieving a high stability for at least 33 h, a high mass activity of 0.
View Article and Find Full Text PDFA general electrocatalyst design for water splitting through generating oxygen vacancies in bimetallic layered double hydroxides by using carbon nitride is proposed. The excellent OER activity of the achieved bimetallic layered double hydroxides is attributed to oxygen vacancies, which reduce the energy barrier of the rate-determining step.
View Article and Find Full Text PDFDeveloping efficient and simple catalysts to reveal the key scientific issues in the epoxidation of ethylene has been a long-standing goal for chemists, whereas a heterogenized molecular-like catalyst is desirable which combines the best aspects of homogeneous and heterogeneous catalysts. Single-atom catalysts can effectively mimic molecular catalysts on account of their well-defined atomic structures and coordination environments. Herein, we report a strategy for selective epoxidation of ethylene, which exploits a heterogeneous catalyst comprising iridium single atoms to interact with the reactant molecules that act analogously to ligands, resulting in molecular-like catalysis.
View Article and Find Full Text PDFHydrogen evolution reaction (HER) in neutral media is of great practical importance for sustainable hydrogen production, but generally suffers from low activities, the cause of which has been a puzzle yet to be solved. Herein, by investigating the synergy between Ru single atoms (RuNC) and RuSe cluster compounds (RuSe) for HER using ab initio molecular dynamics, operando X-ray absorption spectroscopy, and operando surface-enhanced infrared absorption spectroscopy, we establish that the interfacial water governs neutral HER. The rigid interfacial water layer in neutral media would inhibit the transport of HO*/OH* at the electrode/electrolyte interface of RuNC, but the RuSe can promote HO*/OH* transport to increase the number of available HO* on RuNC by disordering the interfacial water network.
View Article and Find Full Text PDFSolar-driven photocatalytic reactions can mildly activate hydrocarbon C-H bonds to produce value-added chemicals. However, the inefficient utilization of photogenerated carriers hinders the application. Here, we report reversible photochromic BiOBr (denoted as -BiOBr) nanosheets that were colored by trapping photogenerated holes upon visible light irradiation and bleached by water oxidation to generate hydroxyl radicals, demonstrating enhanced carrier separation and water oxidation.
View Article and Find Full Text PDFHeterojunctions modulated internal electric field (IEF) usually result in suboptimal efficiencies in carrier separation and utilization because of the narrow IEF distribution and long migration paths of photocarriers. In this work, we report distinctive bismuth oxyhydroxide compound nanorods (denoted as BOH NRs) featuring surface-exposed open channels and a simple chemical composition; by simply modifying the bulk anion layers to overcome the limitations of heterojunctions, the bulk IEF could be readily modulated. Benefiting from the unique crystal structure and the localization of valence electrons, the bulk IEF intensity increases with the atomic number of introduced halide anions.
View Article and Find Full Text PDFACS Appl Mater Interfaces
August 2021
Lithium oxygen (Li-O) batteries have shown great potential as new energy-storage devices due to the high theoretical energy density. However, there are still substantial problems to be solved before practical application, including large overpotential, low energy efficiency, and poor cycle life. Herein, we have successfully synthesized a RuO-CoO nanohybrid with a rich oxygen vacancy and large specific surface area.
View Article and Find Full Text PDFIt is still challenging to develop sulfur electrodes for Li-S batteries with high electrical conductivity and fast kinetics, as well as efficient suppression of the shuttling effect of lithium polysulfides. To address such issues, herein, polar MoTe with different phases (2H, 1T, and 1T') were deeply investigated by density functional theory calculations, suggesting that the 1T'-MoTe displays concentrated density of states (DOS) near the Fermi level with high conductivity. By optimization of the synthesis, 1T'-MoTe quantum dots decorated three-dimensional graphene (MTQ@3DG) was prepared to overcome these issues, and it accomplished exceptional performance in Li-S batteries.
View Article and Find Full Text PDFThe slow redox kinetics during cycling process and the serious shuttle effect caused by the solubility of lithium polysulfides (LiPSs) dramatically hinder the practical application of Li-S batteries. Herein, a facile and scalable spray-drying strategy is presented to construct conductive polar Mo C quantum dots-decorated carbon nanotube (CNT) networks (MCN) as an efficient absorbent and electrocatalyst for Li-S batteries. The results reveal that the MCN/S electrode exhibits a high specific capacity of 1303.
View Article and Find Full Text PDFDeveloping novel bifunctional electrocatalysts with advanced oxygen electrocatalytic activity is pivotal for next-generation energy-storage devices. Herein, we present ultrathin oxygen-doped FePSe (FePSe-O) nanosheets by Ar/O plasma treatment, with remarkable surface atom reorganization. Such surface atom reorganization generates multiple crystalline-amorphous interfaces that benefit the kinetics of oxygen evolution reaction, achieving a low overpotential of only 261 mV at 10 mA cm with a small Tafel slope of 41.
View Article and Find Full Text PDFNickel dichalcogenides have received extensive attention as promising noble-metal-free nanocatalysts for a hydrogen evolution reaction. Nonetheless, their catalytic performance is restricted by the sluggish reaction kinetics, limited exposed active sites, and poor conductivity. In this work, we report on an effective strategy to solve those problems by using an as-designed new porous-C/NiSeS nanocatalyst with the NiSeS nanostubs anchored on with porous-carbon skeletons process.
View Article and Find Full Text PDFThe necessity of Earth-abundant low-cost catalysts with activity similar to noble metals such as platinum is indispensable in order to realize the production of hydrogen through electrolysis of water. Herein, we report a relatively low-cost NiAg 3D porous nanocluster catalyst whose activity matches with that of the state-of-the-art Pt/C in 1 M KOH solution. The catalyst is designed on the principle of creating an interface between a metal having a positive Gibbs energy of hydrogen adsorption and a metal of negative Gibbs energy based on the volcano plot, to tune the Gibbs energy of hydrogen adsorption near zero for enhanced hydrogen evolution.
View Article and Find Full Text PDFExploring the highly efficient and durable electrocatalysts for hydrogen evolution reaction (HER) is vitally necessary for sustainable energy conversion and storage system. Herein, we fabricate an interfacial engineered Rh-carbon nitride as advanced electrocatalysts for HER in the acidic and alkaline electrolytes. The interface between Rh nanocrystals and carbon nitride may adjust the electronic structure of Rh, which results in high activity for HER.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2020
Highly active catalysts from the earth-abundant metals are essential to materialize the low-cost production of hydrogen through water splitting. Herein, nickel porous networks codoped with Cu and Fe prepared by thermal reduction of presynthesized Cu, Fe-codoped Ni(OH) nanowires are reported. The sample consists of nanoparticles of ∼80 nm, which form highly porous network clusters of ∼1 μm with a pore size of 10-100 nm.
View Article and Find Full Text PDFSodium-ion batteries have attracted interest as an alternative to lithium-ion batteries because of the abundance and cost effectiveness of sodium. However, suitable anode materials with high-rate and stable cycling performance are still needed to promote their practical application. Herein, three-dimensional Na Ti O nanowire arrays with enriched surface vacancies endowed by phosphorus doping are reported.
View Article and Find Full Text PDFNon-noble element catalysis for hydrogen evolution reaction (HER) is a promising pathway for mass hydrogen production through electrochemical water splitting. In this work, the catalytic performance of metal (alkali, alkali-earth, and transition metal) atoms anchored to silicene was investigated by density functional theory. Results showed that all the studied metal atoms are energetically favorably absorbed on the silicene with large binding energies.
View Article and Find Full Text PDF