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

Unveiling Cutting‐Edge Developments in Electrocatalytic Nitrate‐to‐Ammonia Conversion DOI
Haoran Zhang, Haijian Wang, X. P. Cao

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(16)

Published: Jan. 11, 2024

The excessive enrichment of nitrate in the environment can be converted into ammonia (NH

Language: Английский

Citations

157
Electrochemical nitrate reduction in acid enables high-efficiency ammonia synthesis and high-voltage pollutes-based fuel cells DOI Creative Commons
Rong Zhang, Chuan Li, Huilin Cui

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Dec. 5, 2023

Abstract Most current research is devoted to electrochemical nitrate reduction reaction for ammonia synthesis under alkaline/neutral media while the investigation of acidic conditions rarely reported. In this work, we demonstrate potential TiO 2 nanosheet with intrinsically poor hydrogen-evolution activity selective and rapid conditions. Hybridized iron phthalocyanine, resulting catalyst displays remarkably improved efficiency toward formation owing enhanced adsorption, suppressed hydrogen evolution lowered energy barrier rate-determining step. Then, an alkaline-acid hybrid Zn-nitrate battery was developed high open-circuit voltage 1.99 V power density 91.4 mW cm –2 . Further, environmental sulfur recovery can be powered by above hydrazine-nitrate fuel cell simultaneously hydrazine/nitrate conversion electricity generation. This work demonstrates attractive electrosynthesis broadens field conversion.

Language: Английский

Citations

116
Electrocatalytic Nitrate and Nitrite Reduction toward Ammonia Using Cu2O Nanocubes: Active Species and Reaction Mechanisms DOI Creative Commons
Lichen Bai, Federico Franco,

Janis Timoshenko

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(14), P. 9665 - 9678

Published: April 1, 2024

The electrochemical reduction of nitrate (NO3–) and nitrite (NO2–) enables sustainable, carbon-neutral, decentralized routes to produce ammonia (NH3). Copper-based materials are promising electrocatalysts for NOx– conversion NH3. However, the underlying reaction mechanisms role different Cu species during catalytic process still poorly understood. Herein, by combining quasi in situ X-ray photoelectron spectroscopy (XPS) operando absorption (XAS), we unveiled that is mostly metallic form highly selective NO3–/NO2– On contrary, Cu(I) predominant a potential region where two-electron NO3– NO2– major reaction. Electrokinetic analysis Raman was also used propose possible steps intermediates leading NH3, respectively. This work establishes correlation between performance dynamic changes chemical state Cu, provides crucial mechanistic insights into pathways electrocatalytic reduction.

Language: Английский

Citations

79
Crystal Phase Engineering of Ultrathin Alloy Nanostructures for Highly Efficient Electroreduction of Nitrate to Ammonia DOI Creative Commons
Yunhao Wang,

Fengkun Hao,

Mingzi Sun

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(14)

Published: Jan. 26, 2024

Abstract Electrocatalytic nitrate reduction reaction (NO 3 RR) toward ammonia synthesis is recognized as a sustainable strategy to balance the global nitrogen cycle. However, it still remains great challenge achieve highly efficient production due complex proton‐coupled electron transfer process in NO RR. Here, controlled of RuMo alloy nanoflowers (NFs) with unconventional face‐centered cubic (fcc) phase and hexagonal close‐packed/fcc heterophase for RR reported. Significantly, fcc NFs demonstrate high Faradaic efficiency 95.2% large yield rate 32.7 mg h −1 cat at 0 −0.1 V (vs reversible hydrogen electrode), respectively. In situ characterizations theoretical calculations have unraveled that possess highest d‐band center superior electroactivity, which originates from strong Ru─Mo interactions intrinsic activity phase. The optimal electronic structures supply adsorption key intermediates suppression competitive evolution, further determines remarkable performance. successful demonstration high‐performance zinc‐nitrate batteries suggests their substantial application potential electrochemical energy systems.

Language: Английский

Citations

73
Constructing molecule-metal relay catalysis over heterophase metallene for high-performance rechargeable zinc-nitrate/ethanol batteries DOI Creative Commons
Jingwen Zhou, Yuecheng Xiong, Mingzi Sun

et al.

Proceedings of the National Academy of Sciences, Journal Year: 2023, Volume and Issue: 120(50)

Published: Dec. 8, 2023

Zinc-nitrate batteries can integrate energy supply, ammonia electrosynthesis, and sewage disposal into one electrochemical device. However, current zinc-nitrate still severely suffer from the limited density poor rechargeability. Here, we report synthesis of tetraphenylporphyrin (tpp)-modified heterophase (amorphous/crystalline) rhodium-copper alloy metallenes (RhCu M-tpp). Using RhCu M-tpp as a bifunctional catalyst for nitrate reduction reaction (NO

Language: Английский

Citations

43
RhNi Bimetallenes with Lattice‐Compressed Rh Skin towards Ultrastable Acidic Nitrate Electroreduction DOI
Wei Zhong,

Qing‐Ling Hong,

Xuan Ai

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(23)

Published: Feb. 26, 2024

Harvesting recyclable ammonia (NH

Language: Английский

Citations

41
Screening of Intermetallic Compounds Based on Intermediate Adsorption Equilibrium for Electrocatalytic Nitrate Reduction to Ammonia DOI
Chaoqun Ma,

Huaifang Zhang,

Jing Xia

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(29), P. 20069 - 20079

Published: July 10, 2024

Electrocatalytic nitrate (NO

Citations

37
Electrocatalytic Nitrate Reduction on Metallic CoNi‐Terminated Catalyst with Industrial‐Level Current Density in Neutral Medium DOI
Yingying Wei, Jingjing Huang, Hong Chen

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(30)

Published: May 9, 2024

Abstract Green ammonia synthesis through electrocatalytic nitrate reduction reaction (eNO 3 RR) can serve as an effective alternative to the traditional energy‐intensive Haber‐Bosch process. However, achieving high Faradaic efficiency (FE) at industrially relevant current density in neutral medium poses significant challenges eNO RR. Herein, with guidance of theoretical calculation, a metallic CoNi‐terminated catalyst is successfully designed and constructed on copper foam, which achieves FE up 100% under industrial‐level very low overpotential (−0.15 V versus reversible hydrogen electrode) medium. Multiple characterization results have confirmed that maintained metal atom‐terminated surface interaction atoms plays crucial role reducing density. By constructing homemade gas stripping absorption device, complete conversion process for high‐purity ammonium products demonstrated, displaying potential practical application. This work suggests sustainable promising toward directly converting nitrate‐containing pollutant solutions into nitrogen fertilizers.

Language: Английский

Citations

36
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 International Edition, Journal Year: 2024, Volume and Issue: 63(18)

Published: March 7, 2024

Electrochemical reduction of nitrate to ammonia (NO

Language: Английский

Citations

34
Electronic Structure Design of Transition Metal-Based Catalysts for Electrochemical Carbon Dioxide Reduction DOI Creative Commons
Liang Guo, Jingwen Zhou, Fu Liu

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(14), P. 9823 - 9851

Published: March 28, 2024

With the increasingly serious greenhouse effect, electrochemical carbon dioxide reduction reaction (CO2RR) has garnered widespread attention as it is capable of leveraging renewable energy to convert CO2 into value-added chemicals and fuels. However, performance CO2RR can hardly meet expectations because diverse intermediates complicated processes, necessitating exploitation highly efficient catalysts. In recent years, with advanced characterization technologies theoretical simulations, exploration catalytic mechanisms gradually deepened electronic structure catalysts their interactions intermediates, which serve a bridge facilitate deeper comprehension structure-performance relationships. Transition metal-based (TMCs), extensively applied in CO2RR, demonstrate substantial potential for further modulation, given abundance d electrons. Herein, we discuss representative feasible strategies modulate catalysts, including doping, vacancy, alloying, heterostructure, strain, phase engineering. These approaches profoundly alter inherent properties TMCs interaction thereby greatly affecting rate pathway CO2RR. It believed that rational design modulation fundamentally provide viable directions development toward conversion many other small molecules.

Language: Английский

Citations

33