Crystal defect engineering of Bi2Te3 nanosheets by Ce doping for efficient electrocatalytic nitrogen reduction

Nan, Jianli; Liu, Yongqin; Chao, Daiyong; Fang, Youxing; Dong, Shaojun

doi:10.1007/s12274-022-5319-x

Cited by 18 publications

(8 citation statements)

References 60 publications

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“…This breakthrough in ENRR performance can be attributed to the addition of Ce, which efficaciously modulate the electronic structure, causing crystalline phase disordered in electrocatalysts as well as building strong synergistic effect with Cu. 58 Furthermore, more oxygen vacancies are created, which can boost the NRR reaction kinetics by accelerating electron migration and conduction. 58,59 The LSV curves in Figure S10f powerfully confirm that the HER is effectively suppressed when Ce is involved in the fabrication of electrocatalysts.…”

Section: Enrr Performancementioning

confidence: 99%

“…58 Furthermore, more oxygen vacancies are created, which can boost the NRR reaction kinetics by accelerating electron migration and conduction. 58,59 The LSV curves in Figure S10f powerfully confirm that the HER is effectively suppressed when Ce is involved in the fabrication of electrocatalysts. Nonetheless, Cu 0.10 Ce 0.15 -PC poses worse ENRR behaviors.…”

Section: Enrr Performancementioning

confidence: 99%

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Solar Self-Driven Electrocatalytic Reduction of N₂ Directly to CO₂-Free Generation of Ammonia on a Coupled Ce-Mediated Cu/Porous Carbon Electrode

Li,

Qiao

et al. 2024

ACS Sustainable Chem. Eng.

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Reduction of nitrogen to ammonia under mild conditions is recognized as one key step in the NH3-economy. The Haber–Bosch process, the typical ammonia production technique, is energy-intensive and high carbon-emitting. Intense efforts have been devoted to searching for sustainable options for decarbonized ammonia generation. Wherein, the electrocatalytic nitrogen fixation route driven by renewable energy is extremely anticipated. Herein, the integrated concept for ammonia production powered by direct solar energy is outlined and proposed. Responding to the limited yield rate and reasonable Faraday efficiency in ammonia synthesis, non-precious Cu-electrocatalysts with porous carbon as substrates are fabricated and Ce is introduced as a modulator which could facilitate electron conduction and nitrogen trapping. By optimizing the proportion of metal sources, strongly synergistic metallic effect of Ce and Cu is structured, further enhancing nitrogen reduction performance of electrocatalysts and inhibiting hydrogen evolution reaction. A satisfactory NH3 yield rate of 30.60 ± 3.04 μg h–1 mgcat –1 is achieved at −0.3 V vs reversible hydrogen electrode (RHE) in 0.1 M KOH and the corresponding FE is about 8.20 ± 0.22%. The solar self-driven NH3 generation system presents a total yield of 104 μg mgcat –1 and a solar-to-ammonia efficiency of 1% at ∼1.2 V in daylight. This work offers a rational energy-utilizing strategy for the preparation of high-grade NH3 chemical via solar system employing non-precious metal catalysts in zero-carbon emission footprint.

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Section: Enrr Performancementioning

confidence: 99%

Section: Enrr Performancementioning

confidence: 99%

Solar Self-Driven Electrocatalytic Reduction of N₂ Directly to CO₂-Free Generation of Ammonia on a Coupled Ce-Mediated Cu/Porous Carbon Electrode

Li,

Qiao

et al. 2024

ACS Sustainable Chem. Eng.

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“…First, N 2 is difficult to be catalyzed and activated under ambient environments due to the strong bond energy of NN and low N 2 solubility in the aqueous solution. [ 15 ] Second, the highly competitive hydrogen evolution reaction (HER) in aqueous solution would severely restrict the efficiency of NH 3 production, caused by the close working potential between NRR and HER. [ 16 ] Therefore, it is difficult to achieve a high NH 3 yield rate, and it still has a long way to go for realizing industrial eNNR production in the future.…”

Section: Introductionmentioning

confidence: 99%

Post Nitrogen Electrocatalysis Era From Li–N₂Batteries to Zn–N₂Batteries

Meng

Xiong

et al. 2023

Advanced Energy Materials

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ability to deliver high energy density with good environmental friendliness, which are considered as the promising devices for energy storage and conversion in the sustainable human society. [1] Considering the abundance of nitrogen resource in the air, scientists began to shift their research perspective from O 2 or CO 2 to N 2 . With the first presentation of the concept for the Li-N 2 battery in 2017, [2] a new device combining energy conversion and N 2 fixation starts to come into sight. Inspired by this new model, from organic Na/Al-N 2 batteries [3] to aqueous Al/Zn-N 2 batteries, [4] other types of metal-N 2 batteries began to be reported as illustrated in Figure 1. For realizing electrochemical NH 3 production, the reaction path is nitrogen reduction reaction (NRR) during the discharge process for both organic and aqueous metal-N 2 batteries. Based on diverse reaction mechanism under aqueous and organic solution, the subsequent reaction in the charge process for two types of metal-N 2 batteries is different, that is, the nitrogen extraction reaction (NER) for the organic ones and oxygen evolution reaction (OER) for the aqueous ones. Overall, the developments of aqueous metal-N 2 batteries are mainly inspired by the organic metal-N 2 batteries and lag behind their development. Up to now, only part of the reported metal-N 2 batteries shows good electrochemical reversibility, [5] while some are electrochemical irreversible primary batteries that can only be discharged. [6] Unlike organic metal-N 2 batteries, for all the reversible/irreversible aqueous metal-N 2 batteries, NH 3 would be generated during the discharging process. In the meantime, these reversible aqueous metal-N 2 batteries can still be recharged even after the NH 3 releasing. [7] NH 3 plays an important role in maintaining the survival of human beings and the sustainable development for the social economy. First, NH 3 is an important chemical raw material for the production of agricultural nitrogen fertilizer, as well as a key energy storage intermediate and carbon-free energy carrier for the production of fuels, dyes, and other industries articles. [8] Moreover, NH 3 is considered as an excellent hydrogen energy carrier because of its high hydrogen content without carbon element and easy liquefaction for storing and transporting. [9] However, the industrial NH 3 synthesis is still carried out via the Haber-Bosch process developed 100 years ago based on the reaction of N 2 +3H 2 →NH 3 , which proceeds under high working pressure of 20 MPa and heat temperature of 673 K, resulting in Metal-N 2 batteries attract considerable research attention due to the dualfunctional characteristics applied in energy storage and conversion, as well as electrochemical artificial NH 3 yield. Nonetheless, it has been found that not all kinds of metal-N 2 batteries are suitable for combining the above two applications. Herein, recent advances in metal-N 2 batteries are summarized. First, the electrochemical reaction mechanisms for all types of metal-N 2 batteries,...

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“…Ammonia (NH 3 ) as a significant chemical for fertilizer manufacturing also serves as the energy carrier for hydrogen energy development, due to its high hydrogen capacity and remarkable liquefaction ability. − The Haber–Bosch (H–B) process which has been adopted as the mainstream for artificial ammonia production was hailed as a discovery of great magnitude for human society of the last century . Nevertheless, its use is challenging due to its harsh reaction conditions (350–550 °C and 150–350 atm), high energy consumption, and massive carbon dioxide emissions . Therefore, a sustainable and environment-friendly method is urgently in need to reform the NH 3 production process.…”

Section: Introductionmentioning

confidence: 99%

“…6 Nevertheless, its use is challenging due to its harsh reaction conditions (350−550 °C and 150−350 atm), 7 high energy consumption, and massive carbon dioxide emissions. 8 Therefore, a sustainable and environment-friendly method is urgently in need to reform the NH 3 production process. The electrocatalytic nitrogen reduction reaction (NRR) is deemed as an appealing approach for ammonia synthesis with various merits of abundant resources, environmental conservation, electricity actuation, and flexible operation, which has aroused numerous interest in recent years.…”

Section: ■ Introductionmentioning

confidence: 99%

Microfluidic Tailoring of a Ru Nanodots/Carbon Heterocatalyst for Electrocatalytic Nitrogen Fixation

Liu

2023

ACS Appl. Nano Mater.

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The electrocatalytic nitrogen reduction reaction is regarded as a promising environment-friendly method for ammonia synthesis. However, it is hardly satisfactory for meeting industrial demands, owing to its limited activity and selectivity. Herein, a continuous-flow microfluidic platform is developed to efficiently synthesize the Ru nanodots/carbon (Ru/C) hetero-catalyst. By systematically tailoring the reaction dynamics (concentration, temperature, flow ratio, and surfactant), the optimized Ru/C hetero-catalysts show an ultrafine average size (2.16 nm) and high mass loading (3.44 wt %), providing abundant active sites for strong N2 chemisorption. Benefiting from their outstanding nature, the Ru/C hetero-catalysts possess a large ammonia yield of 7.63 μg h–1 cm–2 and a high Faradaic efficiency of 6.51% under the neutral condition (0.1 mol L–1 Na2SO4). Our work opens an innovative pathway for controllable microfluidic tailoring of high-performance hetero-catalysts, which further promotes the development of synthetic ammonia chemical industry.

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Crystal defect engineering of Bi2Te3 nanosheets by Ce doping for efficient electrocatalytic nitrogen reduction

Cited by 18 publications

References 60 publications

Solar Self-Driven Electrocatalytic Reduction of N₂ Directly to CO₂-Free Generation of Ammonia on a Coupled Ce-Mediated Cu/Porous Carbon Electrode

Solar Self-Driven Electrocatalytic Reduction of N₂ Directly to CO₂-Free Generation of Ammonia on a Coupled Ce-Mediated Cu/Porous Carbon Electrode

Post Nitrogen Electrocatalysis Era From Li–N₂Batteries to Zn–N₂Batteries

Microfluidic Tailoring of a Ru Nanodots/Carbon Heterocatalyst for Electrocatalytic Nitrogen Fixation

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Crystal defect engineering of Bi2Te3 nanosheets by Ce doping for efficient electrocatalytic nitrogen reduction

Cited by 18 publications

References 60 publications

Solar Self-Driven Electrocatalytic Reduction of N2 Directly to CO2-Free Generation of Ammonia on a Coupled Ce-Mediated Cu/Porous Carbon Electrode

Solar Self-Driven Electrocatalytic Reduction of N2 Directly to CO2-Free Generation of Ammonia on a Coupled Ce-Mediated Cu/Porous Carbon Electrode

Post Nitrogen Electrocatalysis Era From Li–N2Batteries to Zn–N2Batteries

Microfluidic Tailoring of a Ru Nanodots/Carbon Heterocatalyst for Electrocatalytic Nitrogen Fixation

Contact Info

Product

Resources

About

Solar Self-Driven Electrocatalytic Reduction of N₂ Directly to CO₂-Free Generation of Ammonia on a Coupled Ce-Mediated Cu/Porous Carbon Electrode

Solar Self-Driven Electrocatalytic Reduction of N₂ Directly to CO₂-Free Generation of Ammonia on a Coupled Ce-Mediated Cu/Porous Carbon Electrode

Post Nitrogen Electrocatalysis Era From Li–N₂Batteries to Zn–N₂Batteries