Single‐atom catalyst application in distributed renewable energy conversion and storage

Nickel‐nitrogen‐carbon single‐atom catalysts have attracted widespread interest for CO2 electroreduction but they suffer from poor stability. Herein, we report on the preparation of Cl‐ and N‐doped porous carbon nanosheets with atomically dispersed NiN4Cl active sites (NiN4Cl‐ClNC) through a molten‐salt‐assisted pyrolysis strategy. The optimized NiN4Cl‐ClNC catalyst delivers exceptional CO2 conversion activity with outstanding stability for over 220 h at −0.7 V versus RHE and a high CO Faradaic efficiency of 98.7% at a CO partial current density of 12.4 mA cm‒2. Moreover, NiN4Cl‐ClNC displays a remarkable CO partial current density of approximately 349.4 mA cm−2 in flow‐cell, meeting the requirements of industrial applications. Operando attenuated total reflectance surface‐enhanced infrared absorption spectroscopy and density functional theory calculations are used to understand the outstanding activity and stability. Results reveal that the introduced axial Ni‐Cl bond on the Ni center and Cl─C bond on the carbon support synergetically induce electronic delocalization, which not only stabilizes Ni against leaching but also facilitates the formation of the COOH* intermediate that is found to be the rate‐determining step.

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Stabilizing highly active atomically dispersed NiN₄Cl sites by Cl‐doping for CO₂ electroreduction

Li,

Qi,

Wang

et al. 2023

“…The electrochemical ORR involves a multi‐electron transfer reaction 21,22 . O 2 generates H 2 O 2 through the 2e − path at the cathode 23 . If 4e − transfer occurs, the final product will become H 2 O accordingly 24,25 .…”

Section: Introductionmentioning

confidence: 99%

Research progress of electrocatalysts for the preparation of H₂O₂ by electrocatalytic oxygen reduction reaction

Ren

Dong

Liu

et al. 2023

As an eco‐friendly oxidant and energy carrier, H2O2 is used in various fields. The industrial production of H2O2 mostly depends on the large‐scale anthraquinone oxidation processes with high costs. Electrocatalytic production of H2O2 has attracted attention as a renewable and cost‐effective approach to replace traditional ones. With the recent development of oxygen reduction reaction (ORR) catalysts, remarkable progress in electrocatalysts for electrocatalytic H2O2 production by 2e− ORR has been reported. This review summarizes a detailed overview of the recent progress in 2e− ORR for H2O2 production with the mechanism and various efficient catalysts. The catalysts were divided into three parts: noble metal‐based catalyst, non‐noble metal‐based catalyst, and non‐metal‐based catalyst. The influences of the catalytic activity and selectivity were also discussed. Finally, this review explores the prospects of electrocatalytic 2e− ORR for H2O2 synthesis and potential research directions for electrocatalysts. It aims to offer guidance in designing efficient 2e− ORR electrocatalysts and inspire further innovation in electrocatalytic H2O2 synthesis.

“…Especially, NH 3 is an energy storage intermediate and a carbon‐free energy carrier, with high energy density and no CO 2 emissions from combustion, popping up as a candidate green energy vector 2 . In view of this, to achieve highly efficient ammonia synthesis, researchers have invested a lot of attempts on technical routes such as thermocatalysis, photocatalysis, and electrocatalysis 3–6 . The industrial Haber‐Bosch process, converting the reaction mixture into ammonia, is considered the greatest chemical invention of the 20th century and is the main way to artificially fix nitrogen.…”

Section: Introductionmentioning

confidence: 99%

“…2 In view of this, to achieve highly efficient ammonia synthesis, researchers have invested a lot of attempts on technical routes such as thermocatalysis, photocatalysis, and electrocatalysis. [3][4][5][6] The industrial Haber-Bosch process, converting the reaction mixture into ammonia, is considered the greatest chemical invention of the 20th century and is the main way to artificially fix nitrogen. However, Haber-Bosch process takes place under austere conditions (high temperatures over 400 • C and high pressures of 200-300 bar), consuming large amounts of energy and produces large CO 2 emissions (1.6% of the global total) 7 .…”

mentioning

confidence: 99%

Green and large‐scale production of ammonia: Laser‐driven pyrolysis of nitrogen‐enriched biomass

Wang

et al. 2023

Self Cite

As a vital chemical, ammonia (NH3) plays an irreplaceable role in many fields such as chemical synthesis and energy storage. Green renewable biomass can be converted into biofuels, but its nitrogen resources are underused throughout. Laser‐driven pyrolysis is envisaged to debuts as a bridge to connect them to realize the direct conversion from nitrogen‐rich biomass into ammonia. The pulsed laser‐induced local‐transient thermal effect recognized the biological nitrogen resources conversion, such as cheap and plentiful yeasts, to small gaseous molecules and achieved spectacular ammonia production rate up to 260.4 mg/h, an order of magnitude higher performance than thermochemical ammonia synthesis. Simultaneously, the tiny hot point generated by a low‐energy laser (20 W) guarantees the whole ammonia synthesis reaction system is in a mild environment of low temperature and normal pressure. Additionally, the remaining solid residue after laser‐driven pyrolysis also can be further exploited as a highly active catalyst for electrocatalytic nitrate reduction reaction (NIRR).