Interfacial solar evaporation-based seawater desalination is regarded as one of the most promising strategies to alleviate freshwater scarcity. However, the solar evaporation rate of real seawater is significantly constricted by the ubiquitous salts present in seawater. In addition to the common issue of salt accumulation on the evaporation surface during solar evaporation, strong hydration between salt ions and water molecules leads to a lower evaporation rate for real seawater compared to pure water.
View Article and Find Full Text PDFM-N-C-type single-atom catalysts (SACs) are highly efficient for the electrocatalytic oxygen evolution reaction (OER). And the isolated metal atoms are usually considered real active sites. However, the oxidative structural evolution of coordinated N during the OER will probably damage the structure of M-N-C, hence resulting in a completely different reaction mechanism.
View Article and Find Full Text PDFElectrocatalytic semihydrogenation of acetylene (CH) provides a facile and petroleum-independent strategy for ethylene (CH) production. However, the reliance on the preseparation and concentration of raw coal-derived CH hinders its economic potential. Here, a concave surface is predicted to be beneficial for enriching CH and optimizing its mass transfer kinetics, thus leading to a high partial pressure of CH around active sites for the direct conversion of raw coal-derived CH.
View Article and Find Full Text PDFThe high Faradaic efficiency (FE) of the electrocatalytic deuteration of organics with DO at a large current density is significant for deuterated electrosynthesis. However, the FE and current density are the two ends of a seesaw because of the severe D evolution side reaction at nearly industrial current densities. Herein, we report a combined scenario of a nanotip-enhanced electric field and surfactant-modified interface microenvironment to enable the electrocatalytic deuteration of arylacetonitrile in DO with an 80% FE at -100 mA cm.
View Article and Find Full Text PDFElectrocatalytic reduction of nitrate to ammonia (NRA) has emerged as an alternative strategy for sewage treatment and ammonia generation. Despite excellent performances having been achieved over cobalt-based electrocatalysts, the reaction mechanism as well as veritable active species across a wide potential range are still full of controversy. Here, we adopt CoP, Co, and CoO as model materials to solve these issues.
View Article and Find Full Text PDFThe electrochemical NO reduction reaction (NORR) is a promising approach for both nitrogen cycle regulation and ammonia synthesis. Due to the relatively low concentration of the NO source and poor solubility of NO in solution, mass transfer limitation is a serious but easily overlooked issue. In this work, porous carbon-supported ultrafine Cu clusters grown on Cu nanowire arrays (defined as Cu@Cu/C NWAs) are prepared for low-concentration NORR.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
April 2024
Electrocatalytic nitrate reduction to ammonia is a promising approach in term of pollutant appreciation. Cu-based catalysts performs a leading-edge advantage for nitrate reduction due to its favorable adsorption with *NO. However, the formation of active hydrogen (*H) on Cu surface is difficult and insufficient, leading to the significant generation of by-product NO .
View Article and Find Full Text PDFThe industrial manufacture of epichlorohydrin (ECH) often suffers from excessive corrosive chlorine and multistep processes. Here, we report a one-pot membrane-free Br radical-mediated ECH electrosynthesis. Bromine radicals electro-oxidized from Br ions initiate the reaction and then eliminate HBr from bromohydrin to give ECH and release Br ions for reuse.
View Article and Find Full Text PDFElectrochemical reduction of nitrate waste is promising for environmental remediation and ammonia preparation. This process includes multiple hydrogenation steps, and thus the active hydrogen behavior on the surface of the catalyst is crucial. The crystal phase referred to the atomic arrangements in crystals has a great effect on active hydrogen, but the influence of the crystal phase on nitrate reduction is still unclear.
View Article and Find Full Text PDFElectrocatalytic nitrate (NO) reduction to ammonia (NRA) has emerged as an alternative strategy for effluent treatment and ammonia production. Despite significant advancements that have been achieved in this field, the efficient conversion of low-concentration nitrate to ammonia at low overpotential remains a formidable challenge. This challenge stems from the sluggish reaction kinetics caused by the limited distribution of negatively charged NO in the vicinity of the working electrode and the competing side reactions.
View Article and Find Full Text PDFHeteroatom-doped carbon materials have been widely used in many electrocatalytic reduction reactions. Their structure-activity relationships are mainly explored based on the assumption that the doped carbon materials remain stable during electrocatalysis. However, the structural evolution of heteroatom-doped carbon materials is often ignored, and their active origins are still unclear.
View Article and Find Full Text PDFA key challenge for electrochemical nitrogen reduction reactions (NRR) is the difficulty for conventional catalysts to achieve high currents at low H* coverage to produce appreciable NH . Herein, we specially designed an Au nanoparticle-embedded ZnSe photo-electrode to solve the problem. As-designed photo-electrode achieves excellent NRR performance with a high NH yield (12.
View Article and Find Full Text PDFDecarbonizing N conversion is particularly challenging, but essential for sustainable development of industry and agriculture. Herein, we achieve electrocatalytic activation/reduction of N on X/Fe-N-C (X=Pd, Ir and Pt) dual-atom catalysts under ambient condition. We provide solid experimental evidence that local hydrogen radical (H*) generated on the X site of the X/Fe-N-C catalysts can participate in the activation/reduction of N adsorbed on the Fe site.
View Article and Find Full Text PDFIndustrial manufacturing of ethylene chlorohydrin (ECH) critically requires excess corrosive hydrochloric acid or hypochlorous acid with dealing with massive by-products and wastes. Here we report a green and efficient electrosynthesis of ECH from ethylene oxide (EO) with NaCl over a NiFe O nanosheet anode. Theoretical results suggest that EO and Cl preferentially adsorb on Fe and Ni sites, respectively, collaboratively promoting the ECH synthesis.
View Article and Find Full Text PDFThe direct electrochemical nitric oxide reduction reaction (NORR) is an attractive technique for converting NO into NH with low power consumption under ambient conditions. Optimizing the electronic structure of the active sites can greatly improve the performance of electrocatalysts. Herein, we prepare body-centered cubic RuGa intermetallic compounds (i.
View Article and Find Full Text PDFHighly chemo- and regioselective semihydrogenation of alkynes is significant and challenging for the synthesis of functionalized alkenes. Here, a sequential self-template method is used to synthesize amorphous palladium sulfide nanocapsules (PdS ANCs), which enables electrocatalytic semihydrogenation of terminal alkynes in HO with excellent tolerance to easily reducible groups (e.g.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
June 2022
The electrocatalytic nitrogen oxidation reaction (NOR) to generate nitrate is gaining increasing attention as an alternative approach to the conventional industrial manufacture. But, current progress in NOR is limited by the difficulties in activation and conversion of the strong N≡N bond (941 kJ mol ). Herein, we designed to utilize sulfate to enhance NOR performance over an Rh electrocatalyst.
View Article and Find Full Text PDFAs a metal-free photocatalyst, graphitic carbon nitride (g-CN) shows great potential for photocatalytic water splitting, although its performance is significantly limited by structural defects due to incomplete polymerization. In the present work, we successfully synthesize highly conjugated g-CN nanofoam through an iodide substitution technique. The product possesses a high polymerization degree, low defect density, and large specific surface area; as a result, it achieves a hydrogen evolution rate of 9.
View Article and Find Full Text PDFEngineering high-performance electrocatalysts is of great importance for energy conversion and storage. As an efficient strategy, element doping has long been adopted to improve catalytic activity, however, it has not been clarified how the valence state of dopant affects the catalytic mechanism and properties. Herein, it is reported that the valence state of a doping element plays a crucial role in improving catalytic performance.
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