Understanding the ensemble electrochemistry of random-walk nanoparticles: Improved reaction efficiency and mechanistic insights

Lin, Chin E.; Ye, Jia-Jia; Huang, Xing‐Jiu

doi:10.1016/j.cej.2021.129393

Cited by 8 publications

(2 citation statements)

References 27 publications

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“…Essentially, electroanalysis signals are constrained by the electrode−solution interfacial physical and chemical processes, so it relies not only on the modifiers at the electrode surface but also on the components of the electrolyte solution. 26 Yu et al reported the excellent homogeneous catalytic activity of soluble Fe, Co, and Ni complexes for electrochemical water oxidation. 27 Jiang et al elucidated the outstanding degradation effect of Fe 2+ in H 2 O 2 for phenol.…”

Section: ■ Introductionmentioning

confidence: 99%

Practical Strategy for Arsenic(III) Electroanalysis without Modifier in Natural Water: Triggered by Iron Group Ions in Solution

Cai

Xia

et al. 2023

Anal. Chem.

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Significant progress has been made in nanomaterial-modified electrodes for highly efficient electroanalysis of arsenic(III) (As(III)). However, the modifiers prepared using some physical methods may easily fall off, and active sites are not uniform, causing the potential instability of the modified electrode. This work first reports a promising practical strategy without any modifiers via utilizing only soluble Fe3+ as a trigger to detect trace-level As(III) in natural water. This method reaches an actual detection limit of 1 ppb on bare glassy carbon electrodes and a sensitivity of 0.296 μA ppb–1 with excellent stability. Kinetic simulations and experimental evidence confirm the codeposition mechanism that Fe3+ is preferentially deposited as Fe0, which are active sites to adsorb As(III) and H+ on the electrode surface. This facilitates the formation of AsH3, which could further react with Fe2+ to produce more As0 and Fe0. Meanwhile, the produced Fe0 can also accelerate the efficient enrichment of As0. Remarkably, the proposed sensing mechanism is a general rule for the electroanalysis of As(III) that is triggered by iron group ions (Fe2+, Fe3+, Co2+, and Ni2+). The interference analysis of coexisting ions (Cu2+, Zn2+, Al3+, Hg2+, Cd2+, Pb2+, SO4 2–, NO3 –, Cl–, and F–) indicates that only Cu2+, Pb2+, and F– showed inhibitory effects on As(III) due to the competition of active sites. Surprisingly, adding iron power effectively eliminates the interference of Cu2+ in natural water, achieving a higher sensitivity for 1–15 ppb As(III) (0.487 μA ppb–1). This study provides effective solutions to overcome the potential instability of modified electrodes and offers a practical sensing platform for analyzing other heavy-metal anions.

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Section: ■ Introductionmentioning

confidence: 99%

Practical Strategy for Arsenic(III) Electroanalysis without Modifier in Natural Water: Triggered by Iron Group Ions in Solution

Cai

Xia

et al. 2023

Anal. Chem.

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“…[21] NIE-based reaction mode has been found to significantly increase the reaction efficiency by enhancing the mass transport of reactants. [22][23][24][25] Furthermore, since the spatial and temporal continuum of the reaction at ensemble electrochemistry is broken, this mode can also accelerate reaction kinetics [22] and minimize catalyst degradation. [25] In this work, we find that NIE enabled single nanoparticle electrochemistry can also alter the reaction selectivity by using LaNiO 3 nanocubes (NCs) catalyzed hydrogen peroxide reduction reaction (HPRR) as a model reaction.…”

Section: Introductionmentioning

confidence: 99%

From Ensemble Electrochemistry to Nano‐Impact Electrochemistry: Altered Reaction Selectivity

et al. 2022

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Selective electrochemical production of valued chemicals is of significant importance but remains a great challenge in chemistry. Conventional approaches for enhancing reaction selectivity focus on the improvement of the catalysts themselves. In this work, we systematically studied the reaction kinetics and mass transport behavior of LaNiO3 nanocubes (LaNiO3 NCs) catalyzed hydrogen peroxide reduction reaction (HPRR) at ensemble and single nanoparticle levels using nano‐impact electrochemistry (NIE). We find that the selectivity of HPRR was altered at individual random‐walk nanoparticles as compared to their ensemble counterpart without changing the reaction kinetics, due to the significantly enhanced mass transport at single nanoparticles. This discovery offers the scope of new catalytic approaches for engineering electrochemical reactions in general.

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From Ensemble Electrochemistry to Nano‐Impact Electrochemistry: Altered Reaction Selectivity

et al. 2022

View full text Add to dashboard Cite

Selective electrochemical production of valued chemicals is of significant importance but remains a great challenge in chemistry. Conventional approaches for enhancing reaction selectivity focus on the improvement of the catalysts themselves. In this work, we systematically studied the reaction kinetics and mass transport behavior of LaNiO 3 nanocubes (LaNiO 3 NCs) catalyzed hydrogen peroxide reduction reaction (HPRR) at ensemble and single nanoparticle levels using nano-impact electrochemistry (NIE). We find that the selectivity of HPRR was altered at individual random-walk nanoparticles as compared to their ensemble counterpart without changing the reaction kinetics, due to the significantly enhanced mass transport at single nanoparticles. This discovery offers the scope of new catalytic approaches for engineering electrochemical reactions in general.

show abstract

Understanding the ensemble electrochemistry of random-walk nanoparticles: Improved reaction efficiency and mechanistic insights

Cited by 8 publications

References 27 publications

Practical Strategy for Arsenic(III) Electroanalysis without Modifier in Natural Water: Triggered by Iron Group Ions in Solution

Practical Strategy for Arsenic(III) Electroanalysis without Modifier in Natural Water: Triggered by Iron Group Ions in Solution

From Ensemble Electrochemistry to Nano‐Impact Electrochemistry: Altered Reaction Selectivity

From Ensemble Electrochemistry to Nano‐Impact Electrochemistry: Altered Reaction Selectivity

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