Direct electrosynthesis of hydrogen peroxide (HO) with high production rate and high selectivity through the two-electron oxygen reduction reaction (2eORR) offers a sustainable alternative to the energy-intensive anthraquinone technology but remains a challenge. Herein, a low-coordinated, 2D conductive Zn/Cu metal-organic framework supported on hollow nanocube structures (ZnCu-MOF (H)) is rationally designed and synthesized. The as-prepared ZnCu-MOF (H) catalyst exhibits substantially boosted electrocatalytic kinetics, enhanced HO selectivity, and ultra-high Faradaic efficiency for 2eORR process in both alkaline and neutral conditions.
View Article and Find Full Text PDFPlanning under complex uncertainty often asks for plans that can adapt to changing future conditions. To inform plan development during this process, exploration methods have been used to explore the performance of candidate policies given uncertainties. Nevertheless, these methods hardly enable adaptation by themselves, so extra efforts are required to develop the final adaptive plans, hence compromising the overall decision-making efficiency.
View Article and Find Full Text PDFPhotocatalytic O reduction is an intriguing approach to producing HO, but its efficiency is often hindered by the limited solubility and mass transfer of O in the aqueous phase. Here, we design and fabricate a two-layered (2L) Janus fiber membrane photocatalyst with asymmetric hydrophobicity for efficient photocatalytic HO production. The top layer of the membrane consists of superhydrophobic polytetrafluoroethylene (PTFE) fibers with a dispersed modified carbon nitride (mCN) photocatalyst.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
November 2023
Constructing multifunctional interphases to suppress the rampant Zn dendrite growth and detrimental side reactions is crucial for Zn anodes. Herein, a phytic acid (PA)-ZnAl coordination compound is demonstrated as a versatile interphase layer to stabilize Zn anodes. The zincophilic PA-ZnAl layer can manipulate Zn flux and promote rapid desolvation kinetics, ensuring the uniform Zn deposition with dendrite-free morphology.
View Article and Find Full Text PDFManipulating the coordination environment and electron distribution for heterogeneous catalysts at the atomic level is an effective strategy to improve electrocatalytic performance but remains challenging. Herein, atomically dispersed Fe and Co anchored on nitrogen, phosphorus co-doped carbon hollow nanorod structures (FeCo-NPC) are rationally designed and synthesized. The as-prepared FeCo-NPC catalyst exhibits significantly boosted electrocatalytic kinetics and greatly upshifts the half-wave potential for the oxygen reduction reaction.
View Article and Find Full Text PDFManipulating the intrinsic activity of heterogeneous catalysts at the atomic level is an effective strategy to improve the electrocatalytic performances but remains challenging. Here, atomically dispersed Ni anchored on CeO particles entrenched on peanut-shaped hollow nitrogen-doped carbon structures (-Ni/CeO@NC) is rationally designed and synthesized. The as-prepared -Ni/CeO@NC catalyst exhibits substantially boosted intrinsic activity and greatly reduced overpotential for the electrocatalytic oxygen evolution reaction.
View Article and Find Full Text PDFLithium-sulfur (Li-S) batteries are considered as promising candidates for next-generation energy storage systems in view of the high theoretical energy density and low cost of sulfur resources. The suppression of polysulfide diffusion and promotion of redox kinetics are the main challenges for Li-S batteries. Herein, we design and prepare a novel type of ZnCo-based bimetallic metal-organic framework nanoboxes (ZnCo-MOF NBs) to serve as a functional sulfur host for Li-S batteries.
View Article and Find Full Text PDFZn dendrite growth and undesired parasitic reactions severely restrict the practical use of deep-cycling Zn metal anodes (ZMAs). Herein, we demonstrate an elaborate design of atomically dispersed Cu and Zn sites anchored on N,P-codoped carbon macroporous fibers (denoted as Cu/Zn-N/P-CMFs) as a three-dimensional (3D) versatile host for efficient ZMAs in mildly acidic electrolyte. The 3D macroporous frameworks can alleviate the structural stress and suppress Zn dendrite growth by spatially homogenizing Zn flux.
View Article and Find Full Text PDFHybrid materials, integrating the merits of individual components, are ideal structures for efficient oxygen evolution reaction (OER). However, the rational construction of hybrid structures with decent physical/electrochemical properties is yet challenging. Herein, a promising OER electrocatalyst composed of trimetallic metal-organic frameworks supported over S/N-doped carbon macroporous fibers (S/N-CMF@Fe Co Ni -MOF) via a cation-exchange strategy is delicately fabricated.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2022
Single-atom catalysts (SACs) are being pursued as economical electrocatalysts. However, their low active-site loading, poor interactions, and unclear catalytic mechanism call for significant advances. Herein, atomically dispersed Ni/Co dual sites anchored on nitrogen-doped carbon (a-NiCo/NC) hollow prisms are rationally designed and synthesized.
View Article and Find Full Text PDFThe practical application of Zn-metal anodes (ZMAs) is mainly impeded by the limited lifespan and low Coulombic efficiency (CE) resulting from the Zn dendrite growth and side reactions. Herein, a 3D multifunctional host consisting of N-doped carbon fibers embedded with Cu nanoboxes (denoted as Cu NBs@NCFs) is rationally designed and developed for stable ZMAs. The 3D macroporous configuration and hollow structure can lower the local current density and alleviate the large volume change during the repeated cycling processes.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2021
Mn-based oxides have sparked extensive scientific interest for aqueous Zn-ion batteries due to the rich abundance, plentiful oxidation states, and high output voltage. However, the further development of Mn-based oxides is severely hindered by the rapid capacity decay during cycling. Herein, a two-step metal-organic framework (MOF)-engaged templating strategy has been developed to rationally synthesize heterostructured Mn O -ZnMn O hollow octahedrons (MO-ZMO HOs) for stable zinc ion storage.
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