Efficient and CO-tolerant catalysts for alkaline hydrogen oxidation (HOR) are vital to the commercial application of anion exchange membrane fuel cells (AEMFCs). Herein, a robust Ru-based catalyst (Ru/VOC) with ultrasmall Ru nanoparticles supported on carbon frameworks with atomically dispersed V-O species is prepared elaborately. The catalyst exhibits a remarkable mass activity of 3.
View Article and Find Full Text PDFCancer immunotherapy is revolutionizing oncology. The marriage of nanotechnology and immunotherapy offers a great opportunity to amplify antitumor immune response in a safe and effective manner. Here, electrochemically active Shewanella oneidensis MR-1 can be applied to produce FDA-approved Prussian blue nanoparticles on a large-scale.
View Article and Find Full Text PDFConventional nanozymes often possess low active site density. Pursuing effective strategies for constructing highly active single-atomic nanosystems with maximum atom utilization efficiency is exceptionally attractive. Herein, we develop a facile "missing-linker-confined coordination" strategy to fabricate two self-assembled nanozymes, i.
View Article and Find Full Text PDFSeeking an optimal catalyst to accelerate conversion reaction kinetics of room-temperature sodium-sulfur (RT Na-S) batteries is crucial for improving their electrochemical performance and promoting the practical applications. Herein, theoretical calculations of interfacial interactions of catalysts and polysulfides in terms of the surface adsorption state, interfacial ions migration, and electronic concentration around the Fermi level are systematically proposed as guiding principles of catalyst selection for RT Na-S batteries. As a case, MoN catalyst is accurately selected from transition metal nitrides with different d orbital electrons, and for experiment, it is introduced into the carbon nanofibers as a dual-functioning host (MoN@CNFs).
View Article and Find Full Text PDFThe electroreduction of carbon dioxide (CO) to a liquid product is a viable method for establishing an artificial carbon cycle. Unfortunately, most electrocatalysts' low efficiency and instability prevent them from being used in practical applications. In the current study, we developed ultrasmall Cu nanocrystals embedded in nitrogen-doped carbon nanosheets (Cu/NC-NSs) for selective CO electroreduction by adjusting the potential.
View Article and Find Full Text PDFPotassium ion batteries (KIBs) have attracted great attention recently as a promising large-scale energy storage system by virtue of the bountiful K resource and low standard hydrogen potential of K/K. However, their development is hindered by the limited capacity and inferior cycling stability resulting from the large size of K. Here, a unique vanadium sulfide@carbon nanorod is designed and synthesized for high-performance KIBs.
View Article and Find Full Text PDFMetal phosphides with a high theoretical capacity and low redox potential have been proposed as promising anodes for potassium-ion batteries (PIBs). A reasonable configuration design and introduction of a hollow structure with adequate internal void spaces are effective strategies to overcome the volume expansion of metal phosphides in potassium-ion batteries. Herein, we report a cage-confinement pyrolysis strategy to obtain hollow nanocage-structured nitrogen/phosphorus dual-doped carbon-coated copper phosphide (CuP/CuP@NPC), which exhibits a high initial charge capacity (409 mA h g at 100 mA g) and an outstanding cycle performance (100 mA h g after 5000 cycles at 1000 mA g) as an anode material for PIBs.
View Article and Find Full Text PDFMost previous efforts are devoted to developing transition metals as electrocatalysts guided by the d-band center model. The metals of the s-block of the periodic table have so far received little attention in the application of oxygen reduction reactions (ORR). Herein, a carbon catalyst with calcium (Ca) single atom coordinated with N and O is reported, which displays exceptional ORR activities in both acidic condition (E = 0.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2021
The most active catalysts so far successful in hydrogenation reduction of CO are mainly heterogeneous Cu-based catalysts. The complex coordination environments and multiple active sites in heterogeneous catalysts result in low selectivity of target product, while molecular catalysts with well-defined active sites and tailorable structures allow mechanism-based performance optimization. Herein, we firstly report a single ethylenediaminetetraacetic acid (EDTA) molecular-level immobilized on the surface of carbon nanotube as a catalyst for transferring CO to CH with an excellent performance.
View Article and Find Full Text PDFACS Appl Mater Interfaces
June 2021
Preferential oxidation (PROX) of CO in hydrogen is of great significance for proton exchange membrane fuel cells (PEMFCs) that need a CO-free hydrogen stream as fuel. The key technical problem is developing catalysts that can efficiently remove CO from the H-rich stream within the working temperature range of PEMFCs. Herein, we design a Au/BiO interfacial catalyst for PROX with excellent catalytic performance, which can achieve 100% CO conversion in the PROX reaction over a wide temperature window (70-200 °C) and is perfectly compatible with the operating temperature window (80-180 °C) of PEMFCs.
View Article and Find Full Text PDFThe hydrazine oxidation reaction (HzOR), as a substitute for the sluggish oxygen evolution reaction (OER), is identified as a promising powerfrugal strategy for hydrogen production through water splitting. However, the HzOR activity of the present electrocatalysts is unsatisfying because the work potential is much higher than the theoretical value. Herein, we design a typical Mott-Schottky electrocatalyst consisting of CoP/Co nanoparticles for the HzOR, which exhibits remarkable HzOR activity with ultralow potentials of -69 and 177 mV at 10 and 100 mA cm, respectively.
View Article and Find Full Text PDFJ Colloid Interface Sci
July 2021
Recently, atomically dispersed transition-metal single atom in nitrogen-doped carbon matrix as electrocatalysts has aroused general interest. However, there is no report about vanadium single atom for ORR in the literature. According to d-band center theory for transition-metals, the performance of catalysts is regulated by the electronic structure of the catalytic center which determines the intermediate adsorption kinetics.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2021
Nanomaterials with enzyme-mimicking activity (nanozymes) show potential for therapeutic interventions. However, it remains a formidable challenge to selectively kill tumor cells through enzymatic reactions, while leaving normal cells unharmed. Herein, we present a new strategy based on a single-site cascade enzymatic reaction for tumor-specific therapy that avoids off-target toxicity to normal tissues.
View Article and Find Full Text PDFThe carbonaceous materials with low cost and high safety have been considered as promising anodes for potassium-ion batteries (PIBs). However, it is still a challenge to design a carbonaceous material with long cycle life and high rate performance due to the poor K reaction kinetics. Herein, this article reports a N-doped porous carbon framework (NPCF) with a high nitrogen content of 13.
View Article and Find Full Text PDFIt is known that the main-group metals and their related materials show poor catalytic activity due to a broadened single resonance derived from the interaction of valence orbitals of adsorbates with the broad sp-band of main-group metals. However, Mg cofactors existing in enzymes are extremely active in biochemical reactions. Our density function theory calculations reveal that the catalytic activity of the main-group metals (Mg, Al and Ca) in oxygen reduction reaction is severely hampered by the tight-bonding of active centers with hydroxyl group intermediate, while the Mg atom coordinated to two nitrogen atoms has the near-optimal adsorption strength with intermediate oxygen species by the rise of p-band center position compared to other coordination environments.
View Article and Find Full Text PDFHeterogeneous catalysts facilitate various chemical reactions through the changing of their surface charge density. Herein, we demonstrate an interface engineering strategy to enhance the Ir catalytic performance for oxidation of CO by constructing Ir/CeO nanojunctions using a wet chemical reduction process. The as-prepared Ir/CeO nanojunctions show a complete CO conversion temperature () of 110 °C under 1 vol % CO and retains long-term durability even after 24 h.
View Article and Find Full Text PDFGraphene-based materials still exhibit poor electrocatalytic activities for the hydrogen evolution reaction (HER) although they are considered to be the most promising electrocatalysts. We fabricated a graphene-analogous material displaying exceptional activity towards the HER under acidic conditions with an overpotential (57 mV at 10 mA cm ) and Tafel slope (44.6 mV dec ) superior to previously reported graphene-based materials, and even comparable to the state-of-the art Pt/C catalyst.
View Article and Find Full Text PDFA novel design of no-loading and bifunctional positive electrode, serving as an active material and current collector simultaneously, has been constructed by grass-like nickel foam which shows a battery-type performance and excellent areal specific capacity at 0.540 mA h·cm (over 4500 mF·cm). To obtain a high-performance hybrid capacitor, layered porous carbonaceous composites C/MgO negative electrodes were fabricated, in which MgO nanoparticles serve as "reservoirs" for OH ions from the electrolyte.
View Article and Find Full Text PDFUnlike metals with incomplete d-shells such as Pt and Fe, copper (Cu) with a filled d-electron shell is generally regarded as a sluggish oxygen reduction reaction (ORR) electrocatalyst. However, laccase and other copper enzymes could catalyze the ORR efficiently in nature. Inspired by this, we incorporated Cu-N cofactors (Cu-N and Cu-N) into graphene encapsulated Co frameworks by direct annealing of MOFs with a post etching process.
View Article and Find Full Text PDFDeveloping highly active electrocatalysts with superior durability for both the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in the same electrolyte is a grand challenge to realize the practical application of electrolysis water for producing hydrogen. In this work, an ultrasmall Ru/Cu-doped RuO complex embedded in an amorphous carbon skeleton is synthesized, through thermolysis of Ru-modified Cu-1,3,5-benzenetricarboxylic acid (BTC), as a highly efficient bifunctional catalyst for overall water splitting electrocatalysis. The ultrasmall Ru nanoparticles in the complex expose more activity sites for hydrogen evolution and outperform the commercial Pt/C.
View Article and Find Full Text PDFHeteroatom doping is regarded as a promising method to enhance the sodium storage performance of carbon materials. In this work, a sulfur-enriched N-doped multichannel hollow carbon nanofiber (denoted as S-NCNF) film is prepared through electrospinning technology and heat treatment with sublimed sulfur as the flexible anode for sodium ion batteries (NIBs). The S-NCNF film displays outstanding electrochemical performance, particularly with a high rate capacity (132 mA h g at the current density of 10 A g ) and remarkable long cycling stability (reversible specific capacity of 187 mA h g at 2 A g over 2000 cycles).
View Article and Find Full Text PDFHerein, a simple one-pot way is designed to prepare a type of multifunctional metal-organic framework (MOF)-based hybrid nanogels by in situ hybridization of dopamine monomer in the skeleton of MnCo. The resultant hybrid nanoparticles (named as MCP) show enhanced photothermal conversion efficiency in comparison with pure polydopamine or MnCo nanoparticles (NPs) synthesized under a similar method and, therefore, show great potential for photothermal therapy (PTT) in vivo. The MCP NPs are expected to possess positive magnetic resonance imaging ability due to the high-spin Mn-N6 ( = 5/2) in the skeleton of MnCo.
View Article and Find Full Text PDFManganese (Mn) is generally regarded as not being sufficiently active for the oxygen reduction reaction (ORR) compared to other transition metals such as Fe and Co. However, in biology, manganese-containing enzymes can catalyze oxygen-evolving reactions efficiently with a relative low onset potential. Here, atomically dispersed O and N atoms coordinated Mn active sites are incorporated within graphene frameworks to emulate both the structure and function of Mn cofactors in heme-copper oxidases superfamily.
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