Engineering bimetallic capture sites on hierarchically porous carbon electrode for efficient phosphate electrosorption: multiple active centers and excellent electrochemical properties

Zhang, Peng; He, Mingming; Li, Fukuan; Fang, Dezhi; Li, Kexun; Wang, Hao

doi:10.1039/d2ta07752c

Cited by 33 publications

(4 citation statements)

References 55 publications

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“…As demonstrated in Figure c, the removal capability was promoted by the increasing potential difference (0.8–1.4 V). Higher voltages create a denser EDLC surrounding the electrode surface, encourage phosphate to reach deeper active centers, and accelerate the charge transfer . In particular, L8C2PC exhibited an exceptional phosphate uptake ability of 119.54 mg P g –1 at 1.4 V according to the pseudo-second-order kinetic model (Table S3).…”

Section: Resultsmentioning

confidence: 99%

“…Higher voltages create a denser EDLC surrounding the electrode surface, encourage phosphate to reach deeper active centers, and accelerate the charge transfer. 38 In particular, L8C2PC exhibited an exceptional phosphate uptake ability of 119.54 mg P g −1 at 1.4 V according to the pseudo-second-order kinetic model (Table S3). However, applying more voltage than the electrolysis voltage of water (1.23 V vs SHE) causes side reactions and reduces energy efficiency; therefore, subsequent experiments were performed at 1.2 V. The increase in the number of collisions between phosphate and the L8C2PC electrode can also improve the removal performance.…”

Section: ■ Experimental Sectionmentioning

confidence: 98%

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Unlocking Bimetallic Active Centers via Heterostructure Engineering for Exceptional Phosphate Electrosorption: Internal Electric Field-Induced Electronic Structure Reconstruction

Zhang,

He,

et al. 2023

Environ. Sci. Technol.

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Development of electrode materials exhibiting exceptional phosphate removal performance represents a promising strategy to mitigate eutrophication and meet ever-stricter stringent emission standards. Herein, we precisely designed a novel LaCeO x heterostructure-decorated hierarchical carbon composite (L8C2PC) for highefficiency phosphate electrosorption. This approach establishes an internal electric field within the LaCeO x heterostructure, where the electrons transfer from Ce atoms to neighboring La atoms through superexchange interactions in La−O−Ce coordination units. The modulatory heterostructure endows a positive shift of the d band of La sites and the increase of electron density at Fermi level, promoting stronger orbital overlap and binding interactions. The introduction of oxygen vacancies during the in situ nucleation process reduces the kinetic barrier for phosphate-ion migration and supplies additional active centers. Moreover, the hierarchical carbon framework ensures electrical double-layer capacitance for phosphate storage and interconnected ion migration channels. Such synergistically multiple active centers grant the L8C2PC electrode with high-efficiency record in phosphate electrosorption. As expected, the L8C2PC electrode demonstrates the highest removal capability among the reported electrode materials with a saturation capacity of 401.31 mg P g −1 and a dynamic capacity of 91.83 mg P g −1 at 1.2 V. This electrochemical system also performs well in the dephosphorization in natural water samples with low concentration that enable effluent concentration to meet the first-class discharge standard for China (0.5 mg P L −1 ). This study advances efficient dephosphorization techniques to a new level and offers a deep understanding of the internal electric field that regulates metal orbitals and electron densities in heterostructure engineering.

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Section: Resultsmentioning

confidence: 99%

Section: ■ Experimental Sectionmentioning

confidence: 98%

Unlocking Bimetallic Active Centers via Heterostructure Engineering for Exceptional Phosphate Electrosorption: Internal Electric Field-Induced Electronic Structure Reconstruction

Zhang,

He,

et al. 2023

Environ. Sci. Technol.

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“…The current form has an impact on molecular properties and adsorption behavior. [44][45][46][47][48] We can change the output mode of MS-TENG as needed. AHMP can migrate directionally in the direct current electric field.…”

Section: Charge Regulating Film Formation Mechanismmentioning

confidence: 99%

An Adaptable Charge Source Enabled by Mode‐Switchable TENG for Efficient Self‐Repairing Coating

Yu,

Zhang,

et al. 2024

Adv Funct Materials

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Self‐repairing coatings have received widespread attention due to their ability to repair damaged surfaces. However, film‐forming molecules can only be fixed on the metal surface through relatively weak physical and chemical adsorption. This drawback limits its self‐repairing ability. Here, a mode‐switchable TENG (MS‐TENG) is developed, which has the ability to switch between AC and DC outputs as an adjustable charge source for self‐repairing coatings. Besides the normal sector electrodes of rotational TENG, MS‐TENG has a special design of external electrodes (small extension electrodes on rotator and inner/outer orbit electrodes on stator) and achieves charge accumulation through an excitation circuit and DC output through air breakdown on external electrodes with advantage of the complete release of accumulated charges. Compared with traditional air breakdown TENG, its current output has been improved. In addition, the air breakdown process occurs in the external electrode framework independent of the TENG body. Therefore, the negative impact of air breakdown is suppressed. Finally, MS‐TENG is used to achieve rapid electrostatic adsorption of charged film‐forming molecules through charge injection. MS‐TENG as a charge source effectively improves the performance of self‐repairing coatings, with a corrosion inhibition rate of 96.9%.

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“…Furthermore, MOF-derived porous metal/carbon composites have adjustable structures and large porosity . Their unique porous structures prominently increase the accessible adsorption sites and ensure the availability of active centers. , Importantly, the periodic network structure of the precursor connected by metal nodes and organic ligands ensures a uniform distribution of metal active sites in the derived carbon framework. In order to obtain porous carbon materials with atomically dispersed Fe–N active sites, bimetallic MOF carbonization can be a direct and effective method.…”

Section: Introductionmentioning

confidence: 99%

Uniformly Dispersed Fe–N Active Centers on Hierarchical Carbon Electrode for High-Performance Capacitive Deionization: Plentiful Adsorption Sites and Conductive Electron Transfer

Liu,

Zhang,

Wang

et al. 2023

ACS Sustainable Chem. Eng.

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Capacitive deionization (CDI) is a promising desalination technology to meet the growing demand for clean water resources. Carbon-based materials, as one of the most appealing electrode candidates for CDI, are still limited by low adsorption capacity and slow rates. Heteroatom doping of carbonaceous materials is considered a promising strategy for high-performance CDI desalination. Herein, hierarchically porous carbon with uniformly dispersed Fe–N active centers (FeNC) is fabricated by a one-step pyrolysis treatment from a Zn–Fe bimetal–organic framework. The systematic analysis demonstrated that the synergistic effect of the uniformly dispersed Fe and N increased the specific surface area and graphitization degree of the carbonaceous framework. Moreover, the electrochemical analysis confirmed that Fe intervention effectively increased the specific capacitance and reduced the charge-transfer resistance, ensuring a more desirable electrical double-layer capacitor (EDLC) behavior. As expected, FeNC exhibited an excellent electrosorption capacity of 28.88 mg g–1 and a faster rate (1.85 mg g–1 min–1). The results indicated that the introduction of trace Fe can not only modulate the structural properties of carbon materials to provide more accessible adsorption sites but also form Fe–N to accelerate electron transfer. This work provides a profound insight into the crucial role of Fe–N active centers in carbon-based CDI desalination.

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Engineering bimetallic capture sites on hierarchically porous carbon electrode for efficient phosphate electrosorption: multiple active centers and excellent electrochemical properties

Abstract: Excessive phosphate in water bodies has become a major concern because it causes eutrophication and even disrupts the aquatic ecological balance. Electro-assisted adsorption exhibited great potential for wastewater treatment due...

Cited by 33 publications

References 55 publications

Unlocking Bimetallic Active Centers via Heterostructure Engineering for Exceptional Phosphate Electrosorption: Internal Electric Field-Induced Electronic Structure Reconstruction

Unlocking Bimetallic Active Centers via Heterostructure Engineering for Exceptional Phosphate Electrosorption: Internal Electric Field-Induced Electronic Structure Reconstruction

An Adaptable Charge Source Enabled by Mode‐Switchable TENG for Efficient Self‐Repairing Coating

Uniformly Dispersed Fe–N Active Centers on Hierarchical Carbon Electrode for High-Performance Capacitive Deionization: Plentiful Adsorption Sites and Conductive Electron Transfer

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