Regulating the Electrochemical Nitrate Reduction Performance with Controllable Distribution of Unconventional Phase Copper on Alloy Nanostructures DOI Creative Commons
Yuecheng Xiong, Yunhao Wang, Mingzi Sun

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 6, 2024

Abstract Electrochemical nitrate reduction reaction (NO 3 RR) is emerging as a promising strategy for removal and ammonia (NH ) production using renewable electricity. Although great progresses have been achieved, the crystal phase effect of electrocatalysts on NO RR remains rarely explored. Here, epitaxial growth unconventional 2H Cu hexagonal close‐packed ( hcp IrNi template, resulting in formation three IrNiCu@Cu nanostructures, reported. IrNiCu@Cu‐20 shows superior catalytic performance, with NH Faradaic efficiency (FE) 86% at −0.1 (vs reversible hydrogen electrode [RHE]) yield rate 687.3 mmol g −1 h , far better than common face‐centered cubic Cu. In sharp contrast, IrNiCu@Cu‐30 IrNiCu@Cu‐50 covered by shell display high selectivity toward nitrite 2 − ), FE above 60% 0.1 RHE). Theoretical calculations demonstrated that has optimal electronic structures due to highest d‐band center strongest trend lowest energy barriers. The electroactivity originates from abundant low coordination sites surface, which guarantees fast electron transfer accelerate intermediate conversions. This work provides feasible tactic regulate product distribution engineering electrocatalysts.

Language: Английский

Tandem catalysis in electrocatalytic nitrate reduction: Unlocking efficiency and mechanism DOI Creative Commons
Ziyang Wu, Yanhui Song,

Haocheng Guo

et al.

Interdisciplinary materials, Journal Year: 2024, Volume and Issue: 3(2), P. 245 - 269

Published: Feb. 28, 2024

Abstract The electrochemical nitrate reduction reaction (NO 3 RR) holds promise for ecofriendly removal. However, the challenge of achieving high selectivity and efficiency in electrocatalyst systems still significantly hampers mechanism understanding large‐scale application. Tandem catalysts, comprising multiple catalytic components working synergistically, offer promising potential improving NO RR. This review highlights recent progress designing tandem catalysts RR, including noble metal‐related system, transition metal electrocatalysts, pulsed electrocatalysis strategies. Specifically, optimization active sites, interface engineering, synergistic effects between catalyst components, various situ technologies, theory simulations are discussed detail. Challenges opportunities development scaling up RR further discussed, such as stability, durability, mechanisms. By outlining possible solutions future design, this aims to open avenues efficient comprehensive insights into mechanisms energy sustainability environmental safety.

Language: Английский

Citations

26
Metal Doped Unconventional Phase IrNi Nanobranches: Tunable Electrochemical Nitrate Reduction Performance and Pollutants Upcycling DOI
Yuecheng Xiong, Yunhao Wang,

Chi Ching Tsang

et al.

Environmental Science & Technology, Journal Year: 2024, Volume and Issue: 58(24), P. 10863 - 10873

Published: June 6, 2024

Electrochemical nitrate reduction (NO3RR) provides a new option to abate contamination with low carbon footprint. Restricted by competitive hydrogen evolution, achieving satisfied performance in neutral media is still challenge, especially for the regulation of this multielectron multiproton reaction. Herein, facile element doping adopted tune catalytic behavior IrNi alloy nanobranches an unconventional hexagonal close-packed (hcp) phase toward NO3RR. In particular, obtained hcp IrNiCu favor ammonia production and suppress byproduct formation electrolyte indicated situ differential electrochemical mass spectrometry, high Faradaic efficiency (FE) 85.6% large yield rate 1253 μg cm–2 h–1 at −0.4 −0.6 V (vs reversible electrode (RHE)), respectively. contrast, resultant IrNiCo promote nitrite, peak FE 33.1% −0.1 RHE). Furthermore, hybrid electrolysis cell consisting NO3RR formaldehyde oxidation constructed, which are both catalyzed nanobranches. This electrolyzer exhibits lower overpotential holds potential treat polluted air wastewater simultaneously, shedding light on green chemical based contaminate degradation.

Language: Английский

Citations

24
Controlled Synthesis of Unconventional Phase Alloy Nanobranches for Highly Selective Electrocatalytic Nitrite Reduction to Ammonia DOI Creative Commons
Yunhao Wang, Yuecheng Xiong, Mingzi Sun

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(26)

Published: April 22, 2024

Abstract The controlled synthesis of metal nanomaterials with unconventional phases is significant importance to develop high‐performance catalysts for various applications. However, it remains challenging modulate the atomic arrangements nanomaterials, especially alloy nanostructures that involve different metals distinct redox potentials. Here we report general one‐pot IrNi, IrRhNi and IrFeNi nanobranches hexagonal close‐packed (hcp) phase. Notably, as‐synthesized hcp IrNi demonstrate excellent catalytic performance towards electrochemical nitrite reduction reaction (NO 2 RR), superior NH 3 Faradaic efficiency yield rate 98.2 % 34.6 mg h −1 cat (75.5 Ir ) at 0 −0.1 V (vs reversible hydrogen electrode), respectively. Ex/in situ characterizations theoretical calculations reveal Ir−Ni interactions within improve electron transfer benefit both activation active generation, leading a stronger trend NO RR by greatly reducing energy barriers rate‐determining step.

Language: Английский

Citations

20
Co‐Catalytic Metal‐Support Interactions Design on Single‐Atom Alloy for Boosted Electro‐Reduction of Nitrate to Nitrogen DOI
Ziyang Wu, Xuxin Kang, Sen Wang

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(45)

Published: May 28, 2024

Abstract The past decades have seen considerable imbalances in the nitrogen cycle due to excessive use of nitrate agriculture and industry. Electrocatalytic reduction (NO 3 RR) (N 2 ) holds significant potential for addressing pollution wastewater but suffers from nitrite formation sluggish hydrogeneration process. Here a single atom alloy (SAA) catalyst featuring atomically dispersed Ru on 2D Ni metal (Ru 1 Ni), proving remarkable performance − –N conversion (≈93%) N selectivity (≈99%)) through co‐catalytic metal‐support interactions (CMSI) effect is reported. Significantly, SAA achieves NO RR removal capacity as high 11.1 mg L −1 h cm −2 with 20 cycles stability (9 per cycle), surpassing most previously reported works. core boosting lies synergistically promoted activation accelerated hydrogenation oxide intermediates site substrate, respectively, revealed by various situ experiments theoretical simulations. DFT calculations indicate electron transfer substrate more robust interaction between Ru–Ni comparison that Ni–Ni. This work offers resilient methodology rational design highly efficient electrocatalysts CMSI modulation RR, illuminating arena treatment cycle.

Language: Английский

Citations

18
Optimizing Intermediate Adsorption over PdM (M=Fe, Co, Ni, Cu) Bimetallene for Boosted Nitrate Electroreduction to Ammonia DOI
Yuanbo Zhou, Lifang Zhang, Zebin Zhu

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(18)

Published: March 7, 2024

Abstract Electrochemical reduction of nitrate to ammonia (NO 3 RR) is a promising and eco‐friendly strategy for production. However, the sluggish kinetics eight‐electron transfer process poor mechanistic understanding strongly impedes its application. To unveil internal laws, herein, library Pd‐based bimetallene with various transition metal dopants (PdM (M=Fe, Co, Ni, Cu)) are screened learn their structure–activity relationship towards NO RR. The ultra‐thin structure metallene greatly facilitates exposure active sites, metals break electronic balance upshift d‐band center, thus optimizing intermediates adsorption. anisotropic characteristics these make RR activity in order PdCu>PdCo≈PdFe>PdNi>Pd, record‐high NH yield rate 295 mg h −1 cat along Faradaic efficiency 90.9 % achieved neutral electrolyte on PdCu bimetallene. Detailed studies further reveal that moderate N‐species (*NO *NO 2 ) adsorption ability, enhanced activation, reduced HER facilitate We believe our results will give systematic guidance future design catalysts.

Language: Английский

Citations

17
Active Hydrogen for Electrochemical Ammonia Synthesis DOI Creative Commons
Guoqiang Gan, Hong Guo, Wenjun Zhang

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: April 15, 2024

Abstract Electrochemical ammonia synthesis (EAS) presents an attractive alternative to the Haber–Bosch process due benefits of energy saving, low carbon emission, environmental friendliness, and so on. However, competing hydrogen evolution reaction (HER) severely limits yield, selectivity, current efficiency NH 3 . Although accumulation self‐aggregation active (H*) are primary causes HER, it also serves as critical species intermediate for multistep hydrogenation deoxygenation processes. Therefore, sensible regulation H* generation consumption essential enhancing EAS performance. And is significant thoroughly review strategies control. Herein, a comprehensive introduction provide fundamental understanding its role in electrochemical reactions, including generation, conversion, identification, quantification protocols first proposed. In addition, control carefully summarized with particular focus on regulating enhance activity, Faradaic efficiency. Finally, remaining challenges perspectives discussed. This intended offer profound reactions development technology.

Language: Английский

Citations

17
Boosted Nitrate and CO2 Reduction for Urea Electrosynthesis on p-Block Bi Dispersed Ru Alloys DOI

Shiyao Shang,

Wanru Duan, Xue Zeng

et al.

ACS Sustainable Chemistry & Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 10, 2025

Language: Английский

Citations

2
Accelerating proton coupled electron transfer by confined Cu-Ni bimetallic clusters for boosting electrochemical hydrodeoxygenation of nitrate DOI
Jiayi Zhang, Lu Liu, Nan Hu

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125195 - 125195

Published: Feb. 1, 2025

Language: Английский

Citations

2
Subnanometric Nickel Phosphide Heteroclusters with Highly Active Niδ+–Pδ− Pairs for Nitrate Reduction toward Ammonia DOI
Qi Hu, Chunyan Shang, Xinbao Chen

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: March 26, 2025

The development of efficient electrocatalysts for the neutral nitrate reduction reaction (NO3–RR) toward ammonia (NH3) is essential to address environmental issues caused by NO3– but remains considerably challenging owing sluggish kinetics NO3–RR in media. Herein, we report subnanometric heteroclusters with strongly coupled nickel–phosphorus (Ni–P) dual-active sites as boost NO3–RR. Experimental and theoretical results reveal that feature Ni–P promotes electron transfer from Ni P, generating Niδ+–Pδ− active pairs, which Niδ+ species are highly Pδ− tunes interfacial water hydrogen bonding network promote dissociation step accelerate proton during Consequently, NO3–RR, exhibit a large NH3 yield rate 0.61 mmol h–1 cm–2 at −0.8 V versus reversible electrode, 2.8- 3.3-fold larger than those on nanoparticles clusters, respectively, generated exists NH4+ electrolytes. This study offers an approach boosting electrocatalytic reactions multiple intermediates designing sites.

Language: Английский

Citations

2
Selective Urea Electrosynthesis from Nitrate and CO2 on Isolated Copper Alloyed Ruthenium DOI
Fuzhou Wang,

Shiyao Shang,

Zhuohang Li

et al.

ACS Energy Letters, Journal Year: 2024, Volume and Issue: 9(9), P. 4624 - 4632

Published: Aug. 30, 2024

Urea electrosynthesis by coelectrolysis of NO3– and CO2 (UENC) represents a promising method to enable efficient sustainable urea production. In this work, isolated Cu alloyed Ru (Cu1Ru) is developed as highly active selective UENC catalyst. Combined theoretical computations in situ spectroscopic measurements reveal the synergistic effect Cu1–Ru site Ru–Ru on Cu1Ru promote via tandem catalysis pathway, which drives *NO2/CO2 coupling followed *CO2NO2-to-*CO2NH step. The formed *CO2NH then migrates from adjacent promotes *CO2NH⃗*CO2NH2 → *COOHNH2 steps toward generation. Impressively, achieves high performance flow cell, exhibiting yield rate 21.04 mmol h–1 gcat–1 Faradaic efficiency 51.27% at −0.6 V, outperforming most reported catalysts.

Language: Английский

Citations

15