ZIF-supported AuCu nanoalloy for ammonia electrosynthesis from nitrogen and thin air

Lv, Xian‐Wei; Wang, Lu; Wang, Gui‐Chang; Hao, Ran; Ren, Jin‐Tao; Liu, Xiaolu; Duchesne, Paul N.; Liu, Yuping; Li, Wei; Yuan, Zhong‐Yong; Ozin, Geoffrey A.

doi:10.1039/d0ta02832k

Cited by 34 publications

(23 citation statements)

References 45 publications

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“…In addition, the total N content (Figure S36a), the total C content (Figure S36b), and the N/C ratio (Figure S37) do not play a decisive part in the NRR electrocatalysis. Also, the MoS 2 /NC-900 catalyst shows the highest C dl value of 35.5 mF cm –2 among the prepared MoS 2 /NC- T samples (Figures S38 and S39), meaning its best capability to expose accessible active sites. , It is very consistent with the highest pyridinic-N ratio of MoS 2 /NC-900. On the basis of the above analysis, it can be preliminarily inferred that the electrocatalytic performance of MoS 2 /NC- T catalysts toward NRR is predominantly controlled by the pyridinic-N–Mo active sites.…”

Section: Resultsmentioning

confidence: 88%

“…A schematic diagram of the customized cell used to acquire electrochemical in situ FTIR spectroscopy is depicted in Figure a, and a photograph of the cell is shown in Figure S51. This monitoring device is composed of a Nicolet iS50 spectrometer equipped with a VeeMAX III variable angle specular reflectance accessory and a electrochemical reaction cell equipped with a CaF 2 bottom . The in situ FTIR tests were performed via time-resolved FTIR spectroscopy procedures .…”

Section: Resultsmentioning

confidence: 99%

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Identifying the Dominant Role of Pyridinic-N–Mo Bonding in Synergistic Electrocatalysis for Ambient Nitrogen Reduction

Liu

Suo

et al. 2021

ACS Nano

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For electrochemical nitrogen reduction reaction (NRR), hybridizing transition metal (TM) compounds with nitrogen-doped carbonaceous materials has been recognized as a promising strategy to improve the activity and stability of electrocatalysts due to the synergistic interaction from the TM–N–C active sites. Nevertheless, up to date, the fundamental mechanism of this so-called synergistic electrocatalysis for NRR is still unclear. Particularly, it remains ambiguous which configuration of N dopants, either pyridinic N or pyrrolic N, when coordinated with the TM, predominately contributes to this synergy. Herein, a self-assembled three-dimensional 1T-phase MoS2 microsphere coupled with N-doped carbon was developed (termed MoS2/NC), showing an impressive NRR performance in neutral medium. The hybridization of MoS2 and N-doped carbon can synergistically enhance the NRR efficiency by optimizing the electron transfer of catalyst. Acidification/blocking/poisoning experiments reveal the decisive role of pyridinic-N–Mo bonding, rather than pyrrolic-N–Mo bonding, in synergistically enhancing NRR electrocatalysis. The electrochemical-based in situ Fourier transform infrared spectroscopy (in situ FTIR) technology provides deep insights into the substantial contribution of pyridinic-N–MoS2 sites to NRR electrocatalysis and further uncover the underlying mechanism (associative pathway) at a molecular level.

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Section: Resultsmentioning

confidence: 88%

Section: Resultsmentioning

confidence: 99%

Identifying the Dominant Role of Pyridinic-N–Mo Bonding in Synergistic Electrocatalysis for Ambient Nitrogen Reduction

Liu

Suo

et al. 2021

ACS Nano

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“…The above composite has been proposed to be a pH-independent, high performance stable electrocatalyst for nitrogen reduction reactions (NRR) in nitrogen-saturated electrolytes. Actually, in an acidic electrolyte with the H 2 content of air, AuCu/ZIF-8 would achieve an unexpected ammonia production rate of 23.3 µg h −1 mgcat −1 amongst all electrocatalysts, which refers to one of the significant steps in industrializing green ammonia [111].…”

Section: Electrosynthesismentioning

confidence: 99%

“…15, x FOR PEER REVIEW 15 of 29 electrocatalysts, which refers to one of the significant steps in industrializing green ammonia[111].…”

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confidence: 99%

Green Synthesis of Zeolitic Imidazolate Frameworks: A Review of Their Characterization and Industrial and Medical Applications

et al. 2022

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Metal organic frameworks (MOF) are a class of hybrid networks of supramolecular solid materials comprising a large number of inorganic and organic linkers, all bound to metal ions in a well-organized fashion. Zeolitic imidazolate frameworks (ZIFs) are a sub-group of MOFs with imidazole as an organic linker to metals; it is rich in carbon, nitrogen, and transition metals. ZIFs combine the classical zeolite characteristics of thermal and chemical stability with pore-size tunability and the rich topological diversity of MOFs. Due to the energy crisis and the existence of organic solvents that lead to environmental hazards, considerable research efforts have been devoted to devising clean and sustainable synthesis routes for ZIFs to reduce the environmental impact of their preparation. Green chemistry is the key to sustainable development, as it will lead to new solutions to existing problems. Moreover, it will present opportunities for new processes and products and, at its heart, is scientific and technological innovation. The green chemistry approach seeks to redesign the materials that make up the basis of our society and our economy, including the materials that generate, store, and transport our energy, in ways that are benign for humans and the environment and that possess intrinsic sustainability. This study covers the principles of green chemistry as used in designing strategies for synthesizing greener, less toxic ZIFs the consume less energy to produce. First, the necessity of green methods in today’s society, their replacement of the usual non-green methods and their benefits are discussed; then, various methods for the green synthesis of ZIF compounds, such as hydrothermally, ionothermally, and by the electrospray technique, are considered. These methods use the least harmful and toxic substances, especially concerning organic solvents, and are also more economical. When a compound is synthesized by a green method, a question arises as to whether these compounds can replace the same compounds as synthesized by non-green methods. For example, is the thermal stability of these compounds (which is one of the most important features of ZIFs) preserved? Therefore, after studying the methods of identifying these compounds, in the last part, there is an in-depth discussion on the various applications of these green-synthesized compounds.

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“…−1 . 35 Due to the unique characteristics such as corrosion resistance under harsh conditions and adjustable performance (shorter distance between active sites facilitates component optimization), high-entropy alloys (HEA) also have been applied in NRR. The HEA are synthesized by controlling the coordination entropy within 5 or more metal elements.…”

Section: Nanoscale Advances Accepted Manuscriptmentioning

confidence: 99%

Nanomaterials for the electrochemical nitrogen reduction reaction under ambient conditions

et al. 2021

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ZIF-supported AuCu nanoalloy for ammonia electrosynthesis from nitrogen and thin air

Abstract: One step towards green ammonia: electrosynthesis of ammonia from nitrogen and thin air over a gold–copper nanoalloy-decorated zeolitic imidazolate framework.

Cited by 34 publications

References 45 publications

Identifying the Dominant Role of Pyridinic-N–Mo Bonding in Synergistic Electrocatalysis for Ambient Nitrogen Reduction

Identifying the Dominant Role of Pyridinic-N–Mo Bonding in Synergistic Electrocatalysis for Ambient Nitrogen Reduction

Green Synthesis of Zeolitic Imidazolate Frameworks: A Review of Their Characterization and Industrial and Medical Applications

Nanomaterials for the electrochemical nitrogen reduction reaction under ambient conditions

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