Lithium/bismuth co-functionalized phosphotungstic acid catalyst for promoting dinitrogen electroreduction with high Faradaic efficiency

Liao, Wanru; Liu, Han-Xuan; Qi, Lu; Liang, Shijing; Luo, Yu; Liu, Fujian; Wang, Xiuyun; Chang, Chun‐Ran; Zhang, Jie; Jiang, Lilong

doi:10.1016/j.xcrp.2021.100557

Cited by 13 publications

(15 citation statements)

References 59 publications

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“…The differential charge density in Figure 5E also confirms the acceptance of glycerol electrons by the Ag@LDH@TiO 2 and LDH@TiO 2 photoanodes. 54 In particular, Ag NP-supported LDH@TiO 2 exhibits dramatically enhanced charge transfer, which provides strong evidence that the Ag NPs have a beneficial effect on glycerol oxidation. The increased electron density on Ag@ LDH@TiO 2 weakens the β−C−O bonds, thus leading to the selective activation of the middle hydroxyl.…”

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confidence: 88%

“…On the surface of Ag@LDH, the adsorption energy was calculated to be −1.15 eV, which is higher than that of the same moiety on the LDH surface (−0.78 eV); this indicates that the Ag NPs enhance the affinity of LDH to the middle hydroxyl group in glycerol, which further proves that Ag NPs improve the secondary hydroxyl group selectivity in glycerin oxidation. The differential charge density in Figure E also confirms the acceptance of glycerol electrons by the Ag@LDH@TiO 2 and LDH@TiO 2 photoanodes . In particular, Ag NP-supported LDH@TiO 2 exhibits dramatically enhanced charge transfer, which provides strong evidence that the Ag NPs have a beneficial effect on glycerol oxidation.…”

Section: Resultssupporting

confidence: 61%

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Mediating the Oxidizing Capability of Surface-Bound Hydroxyl Radicals Produced by Photoelectrochemical Water Oxidation to Convert Glycerol into Dihydroxyacetone

et al. 2022

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Highly selective oxidation of a single specific hydroxyl group in glycerol is attractive but challenging because glycerol contains three similar hydroxyl groups. In this work, we developed a ternary photoanode comprising Ag nanoparticle-supported layered double hydroxide (LDH) nanosheets on TiO2 (denoted Ag@LDH@TiO2) for the glycerol selective oxidation to 1,3-dihydroxyacetone via photoelectrochemical water oxidation under neutral conditions. It was proved that hydroxyl radicals generated by water oxidation were the dominating active oxygen species and oxygen atoms in the main oxidation product came from water. The LDHs and Ag nanoparticles enhanced the selectivity of secondary hydroxyl oxidation, and the Ag nanoparticles further accelerated the corresponding kinetics. The Ag@LDH@TiO2 photoanode exhibited a 1,3-dihydroxyacetone selectivity of 72% at 1.2 V vs reversible hydrogen electrode, which is obviously higher than that of pure TiO2 (23.5%) and surpasses most materials reported thus far. The role of LDHs and Ag nanoparticles in selective oxidation of glycerol was revealed through detailed spectroscopic and computational studies. Specifically, Fourier transform infrared spectroscopy analysis revealed that the middle hydroxyl group is preferentially adsorbed to LDH surfaces, while density function theory calculations verified that the surface-bound hydroxyl radicals mediated dehydrogenation barriers of middle carbon of adsorbed glycerol; the Ag nanoparticles promoted the selective adsorption of middle hydroxyl of glycerol, which further induced its selective oxidation.

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confidence: 88%

Section: Resultssupporting

confidence: 61%

Mediating the Oxidizing Capability of Surface-Bound Hydroxyl Radicals Produced by Photoelectrochemical Water Oxidation to Convert Glycerol into Dihydroxyacetone

et al. 2022

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“…Compared with bare PTA, the FE of Mo‐PTA is increased by 26.5 times after the introduction of Mo species. In addition, our research group has also developed a novel Li/Bi dual‐species co‐functionalized PTA electrocatalyst, [ 34 ] in which the Li and Bi species are precisely anchored on the three‐fold hollow (3‐H) site and the four‐fold hollow (4‐H) site, respectively, to expose more active unsaturated W sites in PTA (Figure 8). The optimal eNRR performance of the prepared LiBi@V O ‐PTA catalyst obtains the ammonia yield rate of 3.59 ± 0.06 mmol NH3 ·g cat –1 ·h –1 and FE of 85% ± 1% at –0.1 V vs .…”

Section: Synthesis Of Ammoniamentioning

confidence: 99%

Facile Synthesis and High‐Value Utilization of Ammonia

et al. 2022

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Comprehensive Summary Ammonia is a key component in fertilizer and the carbon‐free hydrogen carrier. Catalytic ammonia synthesis and utilization have played a central role in the development of chemical engineering. The industrial production of ammonia remains dependent on the energy‐ and carbon‐intensive Haber–Bosch process. A major effort has been devoted to developing robust and efficient catalysts, as well as alternative benign processes. Herein, we detail our endeavors that develop the ammonia synthesis and decomposition catalysts, and utilize the ammonia energy. We firstly discuss the catalysts for ammonia synthesis via dissociative and associative process, and the regulation of catalysts’ properties. Then, we review the burgeoning electrocatalytic nitrogen reduction process, focusing on the enhanced catalytic performances by the regulation of the catalysts and the electrode. Additionally, we provide a novel high‐value utilization of ammonia to achieve the “zero‐carbon” circular economy. The promising catalysts, reactors, and ammonia energy systems have been discussed in detail. We end this Account that offers future research directions and prospects of ammonia. What is the most favorite and original chemistry developed in your research group? Ammonia synthesis catalysts and ammonia energy. How do you get into this specific field? Could you please share some experiences with our readers? I have received my B.S. in 1997. After graduation from college, I have joined Prof. Kemei Wei's group at the National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University. Since 1972, our group has dedicated to the efficient industrial synthesis and high‐value utilization of ammonia. So, I have done much work in this field. I think that the research work should match with the major national demands and global challenges. The researcher should focus on cutting‐edge discoveries and creative work. How do you supervise your students? When the students come in our group, I teach them the norms and standards of academic research and writing. After that, I would formulate the research project based on their motivations, aspirations, and academic background. If they have any problems during the project, I will help them overcome. We discuss termly on their research methods and evaluate their research results. I also encourage the students to prepare in advance for the next steps in their career or further study. What is the most important personality for scientific research? Research integrity. What are your hobbies? What's your favorite book(s)? I like playing badminton and table tennis. My favorite books are history and industry development plan. How do you keep the balance between research and family? The understanding and support from the family are very important. I have increased my efficiency and productivity, and tried alternative schedules.

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“…Figure 4-Energy efficiency of studies that were evaluated as probably reliable and reliable31,33,[35][36][37][38]49,50,[52][53][54][55][56][57][58][59][60][61][62] -There are four intervals between the lines: below 20% line is interval 1 which the articles are not practically relevant however might fins use in some niche markets, between line one and two (20-35%) is interval 2 that is probably practically relevant, between line…”

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confidence: 99%

Low-temperature electrochemical ammonia synthesis: measurement reliability and comparison to Haber-Bosch in terms of energy efficiency

Rezai

Læsaa

Şahin

et al. 2023

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Recently several studies paved a way to nearly 100% selectivity of the electrochemical ammonia synthesis (EAS), which had been identified earlier as a main challenge. These results motivated us to benchmark the energy efficiency (EE) of EAS against the Haber-Bosch process. We present a method to calculate EE of EAS, which can be used by a broader audience. EAS studies historically suffered from reliability issues, and to avoid benchmarking of false-positive results, we established a method to calculate a reliability indicator to assess the measurement reliability of a published work. We used the indicator to evaluate the studies published in 2020, 2021 and 2022. We calculated the EE of EAS for works that were assessed as reliable with our indicator. We identified and discussed several promising systems and strategies enabling higher selectivity and EE. The EE of some aqueous EAS reports are up to 55%, and non-aqueous are below 15%.

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Lithium/bismuth co-functionalized phosphotungstic acid catalyst for promoting dinitrogen electroreduction with high Faradaic efficiency

Cited by 13 publications

References 59 publications

Mediating the Oxidizing Capability of Surface-Bound Hydroxyl Radicals Produced by Photoelectrochemical Water Oxidation to Convert Glycerol into Dihydroxyacetone

Mediating the Oxidizing Capability of Surface-Bound Hydroxyl Radicals Produced by Photoelectrochemical Water Oxidation to Convert Glycerol into Dihydroxyacetone

Facile Synthesis and High‐Value Utilization of Ammonia

Low-temperature electrochemical ammonia synthesis: measurement reliability and comparison to Haber-Bosch in terms of energy efficiency

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