Highly Effective and Durable Integrated-Chainmail Electrode for H Production through HS Electrolysis.

HS is a prevalent yet toxic gas commonly encountered during fossil fuel extraction, whose electrolysis not only addresses pollution concerns but also facilitates hydrogen production. However, the advancement of HS electrolysis at high current density has been impeded by the lack of stable and highly active electrodes that can endure the corrosive effects of HS poisoning. Herein, we present an integrated-chainmail electrode that features dual-level chainmail structure with graphene encapsulating nickel foam (Ni@NC foam) to enhance HS electrolysis.

Electrosynthesis of NH from NO with ampere-level current density in a pressurized electrolyzer.

Electrocatalytic NO reduction reaction (NORR) offers a promising route for sustainable NH synthesis along with removal of NO pollutant. However, it remains a great challenge to accomplish both high NH production rate and long duration to satisfy industrial application demands. Here, we report an in situ-formed hierarchical porous Cu nanowire array monolithic electrode ensembled in a pressurized electrolyzer to regulate NORR reaction kinetics and thermodynamics, which delivers an industrial-level NH partial current density of 1007 mA cm with Faradaic efficiency of 96.

MoS-confined Rh-Zn atomic pair boosts photo-driven methane carbonylation to acetic acid.

Direct carbonylation of CH to CHCOOH provides a promising pathway for upgrading of natural gas to transportable liquid chemicals, in which high-efficiency CH activation and controllable C-C coupling are both critical but challenging. Herein, we report that highly efficient photo-driven carbonylation of CH with CO and O to CHCOOH is achieved over MoS-confined Rh-Zn atomic-pair in conjunction with TiO. It delivers a high CHCOOH productivity of 152.

Two-Dimensional Catalysts: From Model to Reality.

Two-dimensional (2D) materials have been utilized broadly in kinds of catalytic reactions due to their fully exposed active sites and special electronic structure. Compared with real catalysts, which are usually bulk or particle, 2D materials have more well-defined structures. With easily identified structure-modulated engineering, 2D materials become ideal models to figure out the catalytic structure-function relations, which is helpful for the precise design of catalysts.

Ambient-condition acetylene hydrogenation to ethylene over WS-confined atomic Pd sites.

Ambient-condition acetylene hydrogenation to ethylene (AC-AHE) is a promising process for ethylene production with minimal additional energy input, yet remains a great challenge due to the difficulty in the coactivation of acetylene and H at room temperature. Herein, we report a highly efficient AC-AHE process over robust sulfur-confined atomic Pd species on tungsten sulfide surface. The catalyst exhibits over 99% acetylene conversion with a high ethylene selectivity of 70% at 25 C, and a record space-time yield of ethylene of 1123 mol mol h under ambient conditions, which is nearly four times that of the typical PdAg/AlO catalyst, and exhibiting superior stability of over 500 h.

Full-Spectrum Light-Harvesting Solar Thermal Electrocatalyst Boosts Oxygen Evolution.

Enabling high-efficiency solar thermal conversion (STC) at catalytic active site is critical but challenging for harnessing solar energy to boost catalytic reactions. Herein, we report the direct integration of full-spectrum STC and high electrocatalytic oxygen evolution activity by fabricating a hierarchical nanocage architecture composed of graphene-encapsulated CoNi nanoparticle. This catalyst exhibits a near-complete 98 % absorptivity of solar spectrum and a high STC efficiency of 97 %, which is superior than previous solar thermal catalytic materials.

High-Pressure Electro-Fenton Driving CH Conversion by O at Room Temperature.

Electrochemical conversion of CH to easily transportable and value-added liquid fuels is highly attractive for energy-efficient CH utilization, but it is challenging due to the low reactivity and solubility of CH in the electrolyte. Herein, we report a high-pressure electro-Fenton (HPEF) strategy to establish a hetero-homogeneous process for the electrocatalytic conversion of CH by O at room temperature. In combination with elevation of reactant pressure to accelerate reaction kinetics, it delivers an unprecedented HCOOH productivity of 11.

Edge-rich molybdenum disulfide tailors carbon-chain growth for selective hydrogenation of carbon monoxide to higher alcohols.

Selective hydrogenation of carbon monoxide (CO) to higher alcohols (COH) is a promising non-petroleum route for producing high-value chemicals, in which precise regulations of both C-O cleavage and C-C coupling are highly essential but remain great challenges. Herein, we report that highly selective CO hydrogenation to COH is achieved over a potassium-modified edge-rich molybdenum disulfide (MoS) catalyst, which delivers a high CO conversion of 17% with a superior COH selectivity of 45.2% in hydrogenated products at 240 °C and 50 bar, outperforming previously reported non-noble metal-based catalysts under similar conditions.

Boosting CO Hydrogenation to Formate over Edge-Sulfur Vacancies of Molybdenum Disulfide.

Synthesis of formate from hydrogenation of carbon dioxide (CO ) is an atom-economic reaction but is confronted with challenges in developing high-performance non-precious metal catalysts for application of the process. Herein, we report a highly durable edge-rich molybdenum disulfide (MoS ) catalyst for CO hydrogenation to formate at 200 °C, which delivers a high selectivity of over 99 % with a superior turnover frequency of 780.7 h surpassing those of previously reported non-precious metal catalysts.

Membrane Electrode Assembly for Electrocatalytic CO Reduction: Principle and Application.

Electrocatalytic CO reduction reaction (CO RR) in membrane electrode assembly (MEA) systems is a promising technology. Gaseous CO can be directly transported to the cathode catalyst layer, leading to enhanced reaction rate. Meanwhile, there is no liquid electrolyte between the cathode and the anode, which can help to improve the energy efficiency of the whole system.

Evolution of Stabilized 1T-MoS by Atomic-Interface Engineering of 2H-MoS /Fe-N towards Enhanced Sodium Ion Storage.

Metallic conductive 1T phase molybdenum sulfide (MoS ) has been identified as promising anode for sodium ion (Na ) batteries, but its metastable feature makes it difficult to obtain and its restacking during the charge/discharge processing result in part capacity reversibility. Herein, a synergetic effect of atomic-interface engineering is employed for constructing 2H-MoS layers assembled on single atomically dispersed Fe-N-C (SA Fe-N-C) anode material that boosts its reversible capacity. The work-function-driven-electron transfer occurs from SA Fe-N-C to 2H-MoS via the Fe-S bonds, which enhances the adsorption of Na by 2H-MoS , and lays the foundation for the sodiation process.

Surface-Preferred Crystal Plane Growth Enabled by Underpotential Deposited Monolayer toward Dendrite-Free Zinc Anode.

Aqueous Zn batteries with ideal energy density and absolute safety are deemed the most promising candidates for next-generation energy storage systems. Nevertheless, stubborn dendrite formation and notorious parasitic reactions on the Zn metal anode have significantly compromised the Coulombic efficiency (CE) and cycling stability, severely impeding the Zn metal batteries from being deployed in the proposed applications. Herein, instead of random growth of Zn dendrites, a guided preferential growth of planar Zn layers is accomplished via atomic-scale matching of the surface lattice between the hexagonal close-packed (hcp) Zn(002) and face-centered cubic (fcc) Cu(100) crystal planes, as well as underpotential deposition (UPD)-enabled zincophilicity.

Highly efficient ethylene production via electrocatalytic hydrogenation of acetylene under mild conditions.

Renewable energy-based electrocatalytic hydrogenation of acetylene to ethylene (E-HAE) under mild conditions is an attractive substitution to the conventional energy-intensive industrial process, but is challenging due to its low Faradaic efficiency caused by competitive hydrogen evolution reaction. Herein, we report a highly efficient and selective E-HAE process at room temperature and ambient pressure over the Cu catalyst. A high Faradaic efficiency of 83.

Electron penetration triggering interface activity of Pt-graphene for CO oxidation at room temperature.

Achieving CO oxidation at room temperature is significant for gas purification but still challenging nowadays. Pt promoted by 3d transition metals (TMs) is a promising candidate for this reaction, but TMs are prone to be deeply oxidized in an oxygen-rich atmosphere, leading to low activity. Herein we report a unique structure design of graphene-isolated Pt from CoNi nanoparticles (PtǀCoNi) for efficiently catalytic CO oxidation in an oxygen-rich atmosphere.

Highly efficient conversion of surplus electricity to hydrogen energy via polysulfides redox.

Decoupled electrolysis of water is a promising strategy for peak load regulation of electricity. The key to developing this technology is to construct decoupled devices containing stable redox mediators and corresponding efficient catalysts, which remains a considerable challenge. Herein, we designed a high-performance device, using polysulfides as mediators and graphene-encapsulated CoNi as catalysts.

Inactivating SARS-CoV-2 by electrochemical oxidation.

Fully inactivating SARS-CoV-2, the virus causing coronavirus disease 2019, is of key importance for interrupting virus transmission but is currently performed by using biologically or environmentally hazardous disinfectants. Herein, we report an eco-friendly and efficient electrochemical strategy for inactivating the SARS-CoV-2 using formed nickel oxide hydroxide as anode catalyst and sodium carbonate as electrolyte. At a voltage of 5 V, the SARS-CoV-2 viruses can be rapidly inactivated with disinfection efficiency reaching 95% in only 30 s and 99.

Nonuniform Electric Field-Enhanced In-Source Declustering in High-Pressure Photoionization/Photoionization-Induced Chemical Ionization Mass Spectrometry for Operando Catalytic Reaction Monitoring.

Photoionization mass spectrometry (PI-MS) is a powerful and highly sensitive analytical technique for online monitoring of volatile organic compounds (VOCs). However, due to the large difference of PI cross sections for different compounds and the limitation of photon energy, the ability of lamp-based PI-MS for detection of compounds with low PI cross sections and high ionization energies (IEs) is insufficient. Although the ion production rate can be improved by elevating the ion source pressure, the problem of generating plenty of cluster ions, such as [MH]·(HO) ( = 1 and 2) and [M], needs be solved.

Boosting hydrogen evolution on MoS via co-confining selenium in surface and cobalt in inner layer.

The lack of highly efficient, inexpensive catalysts severely hinders large-scale application of electrochemical hydrogen evolution reaction (HER) for producing hydrogen. MoS as a low-cost candidate suffers from low catalytic performance. Herein, taking advantage of its tri-layer structure, we report a MoS nanofoam catalyst co-confining selenium in surface and cobalt in inner layer, exhibiting an ultra-high large-current-density HER activity surpassing all previously reported heteroatom-doped MoS.

Direct transformation of dinitrogen: synthesis of -containing organic compounds via N-C bond formation.

-containing organic compounds are of vital importance to lives. Practical synthesis of valuable -containing organic compounds directly from dinitrogen (N), not through ammonia (NH), is a holy-grail in chemistry and chemical industry. An essential step for this transformation is the functionalization of the activated N units/ligands to generate N-C bonds.

Chain Mail for Catalysts.

Encapsulating transition-metal nanoparticles inside carbon nanotubes (CNTs) or spheres has emerged as a novel strategy for designing highly durable nonprecious-metal catalysts. The stable carbon layer protects the inner metal core from the destructive reaction environment and thus is described as chain mail for catalysts. Electron transfer from the active metal core to the carbon layer stimulates unique catalytic activity on the carbon surface, which has been utilized extensively in a variety of catalytic reaction systems.

Robust Interface Ru Centers for High-Performance Acidic Oxygen Evolution.

RuO is considered as the state-of-the-art electrocatalyst for the oxygen evolution reaction (OER) in acidic media. However, its practical application is largely hindered by both the high reaction overpotential and severe electrochemical corrosion of the active centers. To overcome these limitations, innovative design strategies are necessary, which remains a great challenge.

Tuning the activities of cuprous oxide nanostructures via the oxide-metal interaction.

Despite tremendous importance in catalysis, the design of oxide-metal interface has been hampered by the limited understanding of the nature of interfacial sites and the oxide-metal interaction (OMI). Through construction of well-defined CuO/Pt, CuO/Ag and CuO/Au interfaces, we find that CuO nanostructures (NSs) on Pt exhibit much lower thermal stability than on Ag and Au, although they show the same structure. The activities of these interfaces are compared for CO oxidation and follow the order of CuO/Pt > CuO/Au > CuO/Ag.

Distance Synergy of MoS -Confined Rhodium Atoms for Highly Efficient Hydrogen Evolution.

Perturbing the electronic structure of the MoS basal plane by confining heteroatoms offers the opportunity to trigger in-plane activity for the hydrogen evolution reaction (HER). The key challenge consists of inducing the optimum HER activity by controlling the type and distribution of confined atoms. A distance synergy of MoS -confined single-atom rhodium is presented, leading to an ultra-high HER activity at the in-plane S sites adjacent to the rhodium.