Bimodal nanoporous Pd3Cu1 alloy with restrained hydrogen evolution for stable and high yield electrochemical nitrogen reduction

Pang, Fangjie; Wang, Zhifeng; Zhang, Kai; He, Jia; Zhang, Weiqing; Guo, Chunxian; Ding, Yi

doi:10.1016/j.nanoen.2019.02.019

Cited by 150 publications

(106 citation statements)

References 52 publications

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“…Ammonia production rates of NV‐W 2 N 3 at different potentials (Figure S8, Supporting Information) were shown in Figure a. The highest ammonia production rate of 11.66 ± 0.98 µg h −1 mg cata −1 (3.80 ± 0.32 × 10 −11 mol cm −2 s −1 ) was obtained at −0.2 V versus RHE with the Faradaic efficiency of 11.67 ± 0.93% (Figure b and Table S1, Supporting Information), which are comparable to most of the catalysts in aqueous electrolytes under ambient conditions (Table S2, Supporting Information) . In addition, no N 2 H 4 by‐product was detected under all applied potentials (Figure S9, Supporting Information).…”

Section: Exafs Curve‐fitting Results (Error Bounds (Accuracies) Werementioning

confidence: 75%

Nitrogen Vacancies on 2D Layered W₂N₃: A Stable and Efficient Active Site for Nitrogen Reduction Reaction

et al. 2019

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also aggravate the greenhouse effect. [8] Considering the huge energy consumption of this process and the great potential of NH 3 in future energy systems, protonassisted electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions is becoming increasingly important in realizing low-cost artificial nitrogen fixation. [10][11][12] More importantly, the NRR system can be easily integrated with renewable solar and wind energy into an environmentally benign process for NH 3 production. [2,7] Even though various materials have shown NRR activity in aqueous system, their performance are still hindered by the sluggish reaction kinetics and competitive hydrogen evolution reaction (HER) resulting in poor activity and unsatisfactory selectivity. [13][14][15] The active site for electrochemical NRR needs twofold properties: for one thing, it can accept the lone-pair electrons for effective N 2 adsorption and for the other thing it can donate electrons to antibonding orbitals of dinitrogen molecules for the NN triple-bond activation. [9,13,[16][17][18][19][20] From this perspective, vacancy-engineering materials are ideal for practical applications. [9,16,20] By virtue of the electron redistribution and special chemical properties, the vacancies can provide unique active sites for nitrogen adsorption and activation. [9,[21][22][23][24] Up to now, the most common vacancy that has been studied for NRR is oxygen vacancy. For example, oxygen vacancies on transition metal oxides are active for NRR by enhancing the dinitrogen molecule adsorption. [9,25] However, oxygen vacancy can also improve the HER performance of the host matrix, which may result in poor NRR selectivity. [26][27][28] Alternatively, nitrogen vacancies on transition metal nitride (TMN) are considered as an ideal active site for NRR because of its unique vacancy properties for dinitrogen molecule adsorption and poor HER activity. [29,30] However, the nitrogen vacancy on TMN would be deactivated during NRR process thus results in poor stability. [29] In addition, researchers claim that some TMNs are inactive toward NRR in aqueous system, which is in contrary to theoretical calculations. [31] To gain insightful understanding of NRR mechanism, it is necessary to design TMNs with simplex structure and stable surface vacancies for the linkage of theoretical models and real-world catalysts. 2D material has onefold and fully exposed crystal surface, which is widely used as platform for both theoretical calculations and Electrochemical nitrogen reduction reaction (NRR) under ambient conditions provides an avenue to produce carbon-free hydrogen carriers. However, the selectivity and activity of NRR are still hindered by the sluggish reaction kinetics. Nitrogen Vacancies on transition metal nitrides are considered as one of the most ideal active sites for NRR by virtue of their unique vacancy properties such as appropriate adsorption energy to dinitrogen molecule. However, their catalytic performance is usually limited by the unstable feature. Herein, a new ...

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Section: Exafs Curve‐fitting Results (Error Bounds (Accuracies) Werementioning

confidence: 75%

Nitrogen Vacancies on 2D Layered W₂N₃: A Stable and Efficient Active Site for Nitrogen Reduction Reaction

et al. 2019

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“…In 2019, Pang et al reported bimodal nanoporous Pd 3 Cu 1 alloys with 3D hierarchical interconnected porous structures. [162] The Pd 3 Cu 1 alloys exhibited a high NH 3 yield rate of 39.9 µg mg cat −1 h −1 in 1 m KOH at −0.25 V versus RHE. The high yield rate was achieved because of large surface area and a tailored ratio of 3:1 between NRR-favorable metal Pd and HER-poor metal Cu, albeit a low FE (1.22%).…”

Section: Another Example Of 3d Nanocatalyst In Electrochemical Nrr Ismentioning

confidence: 92%

“…A potential improvement to this system could be the choice of metals because Ag is computationally estimated to be nonreactive toward NRR (Section ). In 2019, Pang et al reported bimodal nanoporous Pd 3 Cu 1 alloys with 3D hierarchical interconnected porous structures . The Pd 3 Cu 1 alloys exhibited a high NH 3 yield rate of 39.9 µg mg cat −1 h −1 in 1 m KOH at −0.25 V versus RHE.…”

Section: Advanced Catalysts For Nitrogen Conversion To Ammoniamentioning

confidence: 99%

Recent Advanced Materials for Electrochemical and Photoelectrochemical Synthesis of Ammonia from Dinitrogen: One Step Closer to a Sustainable Energy Future

Yan

Xia

et al. 2019

Advanced Energy Materials

128

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Ammonia (NH3), an important raw material for chemical industry and agriculture, is also considered to be an intriguing energy storage and transportation media for chemical conversion schemes. The world's primary NH3 supply is based on the natural nitrogen fixation by diazotrophs through an enzymatic nitrogenase process and the industrial nitrogen fixation through a traditional Haber–Bosch process. The natural synthesis of NH3 can hardly meet the rapidly growing global demand. Meanwhile, the industrial NH3 production is still dominated by the high‐temperature and high‐pressure reaction between nitrogen and hydrogen (N2 + 3H2 → 2NH3), requiring intensive energy input and generating massive CO2. Therefore, seeking a breakthrough in the development of catalysts toward efficient ammonia synthesis has become the frontier of energy and chemical conversion schemes. This review summarizes and discusses the recent progress on developing new strategies to optimize the efficiency of NH3 production coupled with renewable energy sources, with a specific focus on electrocatalytic and photoelectrocatalytic conversion of N2 to NH3. The most recent advances in the development of catalytic materials, the design of the reaction systems, and the computational insights for electrochemical and photoelectrochemical ammonia synthesis are covered.

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“…To differentiate, we call it quasi-HEAs. The as-fabricated nanoporous quasi-HEAs possess plentiful dislocations and defects between two neighboring solid solution areas and a high specific surface area, which may be applied in wide chemical fields [41][42][43]. The higher resolution characterization of quasi-HEAs needs to be examined in future work.…”

Section: Resultsmentioning

confidence: 99%

Nanoporous Quasi-High-Entropy Alloy Microspheres

Yang

Wang

et al. 2019

Metals

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High-entropy alloys (HEAs) present excellent mechanical properties. However, the exploitation of chemical properties of HEAs is far less than that of mechanical properties, which is mainly limited by the low specific surface area of HEAs synthesized by traditional methods. Thus, it is vital to develop new routes to fabricate HEAs with novel three-dimensional structures and a high specific surface area. Herein, we develop a facile approach to fabricate nanoporous noble metal quasi-HEA microspheres by melt-spinning and dealloying. The as-obtained nanoporous Cu30Au23Pt22Pd25 quasi-HEA microspheres present a hierarchical porous structure with a high specific surface area of 69.5 m2/g and a multiphase approximatively componential solid solution characteristic with a broad single-group face-centered cubic XRD pattern, which is different from the traditional single-phase or two-phase solid solution HEAs. To differentiate, these are named quasi-HEAs. The synthetic strategy proposed in this paper opens the door for the synthesis of porous quasi-HEAs related materials, and is expected to promote further applications of quasi-HEAs in various chemical fields.

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Bimodal nanoporous Pd3Cu1 alloy with restrained hydrogen evolution for stable and high yield electrochemical nitrogen reduction

Cited by 150 publications

References 52 publications

Nitrogen Vacancies on 2D Layered W₂N₃: A Stable and Efficient Active Site for Nitrogen Reduction Reaction

Nitrogen Vacancies on 2D Layered W₂N₃: A Stable and Efficient Active Site for Nitrogen Reduction Reaction

Recent Advanced Materials for Electrochemical and Photoelectrochemical Synthesis of Ammonia from Dinitrogen: One Step Closer to a Sustainable Energy Future

Nanoporous Quasi-High-Entropy Alloy Microspheres

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Bimodal nanoporous Pd3Cu1 alloy with restrained hydrogen evolution for stable and high yield electrochemical nitrogen reduction

Cited by 150 publications

References 52 publications

Nitrogen Vacancies on 2D Layered W2N3: A Stable and Efficient Active Site for Nitrogen Reduction Reaction

Nitrogen Vacancies on 2D Layered W2N3: A Stable and Efficient Active Site for Nitrogen Reduction Reaction

Recent Advanced Materials for Electrochemical and Photoelectrochemical Synthesis of Ammonia from Dinitrogen: One Step Closer to a Sustainable Energy Future

Nanoporous Quasi-High-Entropy Alloy Microspheres

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Nitrogen Vacancies on 2D Layered W₂N₃: A Stable and Efficient Active Site for Nitrogen Reduction Reaction

Nitrogen Vacancies on 2D Layered W₂N₃: A Stable and Efficient Active Site for Nitrogen Reduction Reaction