Multi-Sites Electrocatalysis in High-Entropy Alloys

Natural nitrogen cycle has been severely disrupted by anthropogenic activities. The overuse of N-containing fertilizers induces the increase of nitrate level in surface and ground waters, and substantial emission of nitrogen oxides causes heavy air pollution. Nitrogen gas, as the main component of air, has been used for mass ammonia production for over a century, providing enough nutrition for agriculture to support world population increase. In the last decade, researchers have made great efforts to develop ammonia processes under ambient conditions to combat the intensive energy consumption and high carbon emission associated with the Haber-Bosch process. Among different techniques, electrochemical nitrate reduction reaction (NO3 RR) can achieve nitrate removal and ammonia generation simultaneously using renewable electricity as the power, and there is an exponential growth of studies in this research direction. Here we provide a timely and comprehensive review on the important progresses of electrochemical NO3 RR, covering the rational design of electrocatalysts, emerging C-N coupling reactions, and advanced energy conversion and storage systems. Moreover, future perspectives are proposed to accelerate the industrialized NH3 production and green synthesis of chemicals, leading to a sustainable nitrogen cycle via prosperous N-based electrochemistry. This article is protected by copyright. All rights reserved.

Electrochemical Nitrate Reduction: Ammonia Synthesis and the Beyond.

In the global trend towards carbon neutrality, sustainable energy conversion and storage technologies are of vital significance to tackle the energy crisis and climate change. However, traditional electrode materials gradually reach their property limits. Two-dimensional (2D) materials featuring large aspect ratios and tunable surface properties exhibit tremendous potential for improving the performance of energy conversion and storage devices. To rationally control the physical and chemical properties for specific applications, defect engineering of 2D materials has been investigated extensively, and is becoming a versatile strategy to promote the electrode reaction kinetics. Simultaneously, exploring the in-depth mechanisms underlying defect action in electrode reactions is crucial to provide profound insight into structure tailoring and property optimization. In this review, we highlight the cutting-edge advances in defect engineering in 2D materials as well as their considerable effects in energy-related applications. Moreover, the confronting challenges and promising directions are discussed for the development of advanced energy conversion and storage systems.

Defect engineering of two-dimensional materials for advanced energy conversion and storage.

Advanced electrocatalysts for complete oxidation of ethylene glycol (EG) in direct EG fuel cells are strongly desired owing to the higher energy efficiency. Herein, Pd-PdSe heterostructural nanosheets (Pd-PdSe HNSs) have been successfully fabricated via one-step approach. These Pd-PdSe HNSs feature unique electronic and geometrical structure, in which unconventional p-d hybridization interaction and tensile strain effect co-exist. Compared with commercial Pd/C and Pd NSs catalysts, Pd-PdSe HNSs display 5.5 (6.6) and 2.5 (2.6) folds enhancement of specific (mass) activity for EG oxidation reaction (EGOR). Especially, the optimum C1 pathway selectivity of Pd-PdSe HNSs reaches 44.3%, illustrating the superior C-C Bond cleavage ability. Electrochemical in situ FTIR spectroscopy and theoretical calculations demonstrate extraordinary p-d hybridization interaction and tensile strain effect could effectively reduce the activation energy of C-C bond breaking and accelerate CO* oxidation, boosting the complete oxidation of EG and improving the catalytic performance.

Extraordinary p-d Hybridization Interaction in Heterostructural Pd-PdSe Nanosheets Boosts C-C Bond Cleavage of Ethylene Glycol Electrooxidation.

Electrocatalytic carbon dioxide reduction reaction (CO2RR) holds significant potential to promote carbon neutrality. However, the selectivity toward multicarbon products in CO2RR is still too low to meet practical applications. Here the authors report the delicate synthesis of three kinds of Ag–Cu Janus nanostructures with {100} facets (JNS‐100) for highly selective tandem electrocatalytic reduction of CO2 to multicarbon products. By controlling the surfactant and reduction kinetics of Cu precursor, the confined growth of Cu with {100} facets on one of the six equal faces of Ag nanocubes is realized. Compared with Cu nanocubes, Ag65–Cu35 JNS‐100 demonstrates much superior selectivity for both ethylene and multicarbon products in CO2RR at less negative potentials. Density functional theory calculations reveal that the compensating electronic structure and carbon monoxide spillover in Ag65–Cu35 JNS‐100 contribute to the enhanced CO2RR performance. This study provides an effective strategy to design advanced tandem catalysts toward the extensive application of CO2RR.

Confined Growth of Silver–Copper Janus Nanostructures with {100} Facets for Highly Selective Tandem Electrocatalytic Carbon Dioxide Reduction

Electrochemical CO2 reduction reaction (CO2RR) is an attractive pathway for closing the anthropogenic carbon cycle and storing intermittent renewable energy by converting CO2 to valuable chemicals and fuels. The production of highly reduced carbon compounds beyond CO and formate, such as hydrocarbon and oxygenate products with higher energy density, is particularly desirable for practical applications. However, the productivity towards highly reduced chemicals is typically limited by high overpotential and poor selectivity due to the multiple electron-proton transfer steps. Tandem catalysis, which is extensively utilized by nature for producing biological macromolecules with multiple enzymes via coupled reaction steps, represents a promising strategy for enhancing the CO2RR performance. Improving the efficiency of CO2RR via tandem catalysis has recently emerged as an exciting research frontier and achieved significant advances. Here we describe the general principles and also considerations for designing tandem catalysis for CO2RR. Recent advances in constructing tandem catalysts, mainly including bimetallic alloy nanostructures, bimetallic heterostructures, bimetallic core-shell nanostructures, bimetallic mixture catalysts, metal-metal organic framework (MOF) and metal-metallic complexes, metal-nonmetal hybrid nanomaterials and copper-free hybrid nanomaterials for boosting the CO2RR performance are systematically summarized. The study of tandem catalysis for CO2RR is still at the early stage, and future research challenges and opportunities are also discussed.

Tandem catalysis in electrochemical CO2 reduction reaction

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Tandem catalysis in electrochemical CO2 reduction reaction