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Fu, Jie

Publications and source records attributed to Fu, Jie.

511 records · Page 29

Creating Frustrated Lewis Pairs in Defective Boron Carbon Nitride for Electrocatalytic Nitrogen Reduction to Ammonia

Abstract The electrocatalytic nitrogen reduction reaction (NRR) on metal‐free catalysts is an attractive alternative to the industrial Haber–Bosch process. However, the state‐of‐the‐art metal‐free electrocatalysts still suffer from low Faraday efficiencies and low ammonia yields. Herein, we present a molecular design strategy to develop a defective boron carbon nitride (BCN) catalyst with the abundant unsaturated B and N atoms as Lewis acid and base sites, which upgrades the catalyst from a single “Lewis acid catalysis” to “frustrated Lewis pairs (FLPs) catalysis.” 14 N 2 / 15 N 2 exchange experiments and density functional theory (DFT) calculations reveal that FLPs can adsorb an N 2 molecule to form a six‐membered ring intermediate, which enables the cleavage of N 2 via a pull–pull effect, thereby significantly reducing the energy barrier to −0.28 eV. Impressively, BCN achieves a high Faraday efficiency of 18.9 %, an ammonia yield of 20.9 μg h −1 mg −1 cat. , and long‐term durability.

Lin, Wenwen↗

Defect-Regulated Frustrated-Lewis-Pair Behavior of Boron Nitride in Ambient Pressure Hydrogen Activation

We report the construction of heterogeneous frustrated Lewis pairs (FLPs) with performance comparable to or surpassing the homogeneous counterparts in H 2 activation is a long-standing challenge. Herein, sterically hindered Lewis acid (“B” center) and Lewis base (“N” center) sites were anchored within the rigid lattice of highly crystalline hexagonal boron nitride (h-BN) scaffolds. The active sites were created via precision defect regulation during the molten-salt-involved (NaNH 2 and NaBH 4 ) h-BN construction procedure. The as-afforded h-BN scaffolds achieved highly efficient H 2 /D 2 activation and dissociation under ambient pressure via FLP-like behavior, and attractive catalytic efficiency in hydrogenation reactions surpassing the current heterogeneous analogues.

36 MATERIALS SCIENCE↗

An ultrastable heterostructured oxide catalyst based on high-entropy materials: A new strategy toward catalyst stabilization via synergistic interfacial interaction

Designing high–performance catalysts that can stabilize catalytic active sites against sintering to deactivation at temperature higher than 900°C is significant but challenging. In this work, we report a new strategy to obtain a transition metal oxide catalyst with high temperature stability for CO oxidation. This is achieved through a synergistic interfacial interaction at the interface of a heterostructure between high– entropy oxides (HEO, high temperature stability) and CuCeO x (catalytic site). The catalytic site (CuCeO x ) for CO oxidation is realized by dissolving an amount of Cu species in HEO into CeO 2 via an entropy–driven mechanochemical process. In situ XRD and HAADF–STEM have confirmed the high temperature stability of the heterostructure CuCeO x –HEO, which can remain its CO oxidation catalytic activity at elevated temperatures. It should be expected that this innovative will offer the potential to the synthesis of catalysts with high temperature stability in industry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗