Efficient interlayer confined nitrate reduction reaction and oxygen generation enabled by interlayer expansion

Zhang, Ye; Xu, Maotian; Xu, Xudong; Li, Xiaoyü; Zhu, Genping; Jia, Gan; Yang, Bingchuan; Yin, Ruilian; Gao, Peng; Ye, Wei

doi:10.1039/d2nr05001c

Cited by 8 publications

(6 citation statements)

References 52 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Simultaneously, it is one of the most widespread water pollutants in the world, which seriously endangers human health and the ecological environment . Consequently, selective conversion of NO 3 – pollutants to high-value-added NH 3 will open up a green pathway for restoring the globally perturbed nitrogen cycle and simultaneously provide a sustainable alternative for the Haber–Bosch process. − …”

mentioning

confidence: 99%

In Situ Construction of Metal–Organic Frameworks as Smart Channels for the Effective Electrocatalytic Reduction of Nitrate at Ultralow Concentrations to Ammonia

et al. 2023

View full text Add to dashboard Cite

Electrochemical conversion of nitrate, a widespread water pollutant, into high-value-added ammonia is a renewable and delocalized route to restore the globally perturbed nitrogen cycle. However, premature desorption of catalytic intermediates and the competitive reaction of hydrogen evolution make the current performance still far from suitable for practical applications. In this work, a Zr-based metal−organic framework (MOF) is in situ constructed at the reaction interface to serve as a smart channel for the highly selective electrocatalytic reduction of nitrate to ammonia. The secondary coordination interaction introduced by the pendant Brønsted acidic groups of MOF not only effectively stabilize the catalytic intermediates to facilitate the overall reaction process but also certainly increase the proton activation barrier to suppress the competing hydrogen evolution reaction. When coupled with a nanocluster active center, the proof-of-concept system achieves simultaneous improvement in three critical parameters, with a nitrate conversion rate of 97.6%, an ammonia selectivity of 95.2%, and a Faradaic efficiency of 91.4% at −1.0 V (vs RHE) under ultralow nitrate concentration conditions. This strategy provides an interesting route for the application of MOFs and paves the way for the removal of nitrate and its reduction to ammonia.

show abstract

mentioning

confidence: 99%

In Situ Construction of Metal–Organic Frameworks as Smart Channels for the Effective Electrocatalytic Reduction of Nitrate at Ultralow Concentrations to Ammonia

et al. 2023

View full text Add to dashboard Cite

show abstract

“…3d , vibrational peaks located at 730 and 1378 cm –1 can be attributed to a N–O bending mode and ν 3 mode of free NO 3 – , respectively 32 , 33 . The intensity of the two peaks gradually increases with reaction time, suggesting the enrichment of NO 3 – on catalyst surface 34 . Two vibrational peaks located at 1216 and 1296 cm –1 synchronously appear at 20 min, which are assigned to *NO 2 and *NH 2 wagging modes, respectively 35 , 36 .…”

Section: Resultsmentioning

confidence: 93%

Kinetically matched C–N coupling toward efficient urea electrosynthesis enabled on copper single-atom alloy

Xu,

Wu,

Zhang

et al. 2023

Nat Commun

Self Cite

View full text Add to dashboard Cite

Chemical C–N coupling from CO2 and NO3–, driven by renewable electricity, toward urea synthesis is an appealing alternative for Bosch–Meiser urea production. However, the unmatched kinetics in CO2 and NO3– reduction reactions and the complexity of C- and N-species involved in the co-reduction render the challenge of C–N coupling, leading to the low urea yield rate and Faradaic efficiency. Here, we report a single-atom copper-alloyed Pd catalyst (Pd4Cu1) that can achieve highly efficient C–N coupling toward urea electrosynthesis. The reduction kinetics of CO2 and NO3– is regulated and matched by steering Cu doping level and Pd4Cu1/FeNi(OH)2 interface. Charge-polarized Pdδ–-Cuδ+ dual-sites stabilize the key *CO and *NH2 intermediates to promote C–N coupling. The synthesized Pd4Cu1-FeNi(OH)2 composite catalyst achieves a urea yield rate of 436.9 mmol gcat.–1 h–1 and Faradaic efficiency of 66.4%, as well as a long cycling stability of 1000 h. In-situ spectroscopic results and theoretical calculation reveal that atomically dispersed Cu in Pd lattice promotes the deep reduction of NO3– to *NH2, and the Pd-Cu dual-sites lower the energy barrier of the pivotal C–N coupling between *NH2 and *CO.

show abstract

“…[6,[8][9]12] For example, oxygen usually exists as functional groups on the surface of carbon materials, which can improve the wettability and benefit for the electrolyte infiltration. [13] Nitrogen in the form of pyridine N, pyrrole N, graphite N, and pyridine nitrogen oxides is one of the most common heteroatom dopants for carbon materials. N atoms can function as electron donors to increase the electronic conductivity of Ndoped carbon materials.…”

Section: Introductionmentioning

confidence: 99%

“…Moreover, doping with non‐metallic heteroatoms such as nitrogen (N), oxygen (O), sulfur (S), and phosphorus (P) have also been proved to be effective to improve the electrochemical performance through providing rich redox‐active sites and enhancing the electronic conductivity of biomass‐derived carbon [6,8–9,12] . For example, oxygen usually exists as functional groups on the surface of carbon materials, which can improve the wettability and benefit for the electrolyte infiltration [13] . Nitrogen in the form of pyridine N, pyrrole N, graphite N, and pyridine nitrogen oxides is one of the most common heteroatom dopants for carbon materials.…”

Section: Introductionmentioning

confidence: 99%

Biomass‐Derived Carbon Materials for Electrochemical Energy Storage

Bai,

Zhang,

Rong

et al. 2024

Chemistry A European J

View full text Add to dashboard Cite

The environmental impact from the waste disposal has been widely concerned around the world. The conversion of wastes to useful resources is important for the sustainable society. As a typical family of wastes, biomass materials basically composed of collagen, protein and lignin, are considered as useful resources for recycle and reuse. In recent years, the development of carbon material derived from biomasses, such as plants, crops, animals and their application in electrochemical energy storage have attracted extensive attention. Through the selection of the appropriate biomass, the optimization of the activation method and the control of the pyrolysis temperatures, carbon materials with desired features, such as high‐specific surface area, variable porous framework, and controllable heteroatom‐doping have been fabricated. Herein, this review summarized the preparation methods, morphologies, heteroatoms doping in the plant/animal‐derived carbonaceous materials, and their application as electrode materials for secondary batteries and supercapacitors, and as electrode support for lithium‐sulfur batteries. The challenges and prospects for the controllable synthesis and large‐scale application of biomass‐derived carbonaceous materials have also been outlooked.

show abstract

Efficient interlayer confined nitrate reduction reaction and oxygen generation enabled by interlayer expansion

Abstract: Electrochemically converting nitrate ions back to ammonia not only can eliminate water pollution, but also obtain valuable ammonia without serious carbon footprint, which is deemed as an efficient supplement to...

Cited by 8 publications

References 52 publications

In Situ Construction of Metal–Organic Frameworks as Smart Channels for the Effective Electrocatalytic Reduction of Nitrate at Ultralow Concentrations to Ammonia

In Situ Construction of Metal–Organic Frameworks as Smart Channels for the Effective Electrocatalytic Reduction of Nitrate at Ultralow Concentrations to Ammonia

Kinetically matched C–N coupling toward efficient urea electrosynthesis enabled on copper single-atom alloy

Biomass‐Derived Carbon Materials for Electrochemical Energy Storage

Contact Info

Product

Resources

About