APPLIED SURFACE SCIENCE
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2021
·
IF 6.707
Lijia Dong,Shengbo Li,Yefei Jin,Baowei Hu,Guodong Sheng
In this paper, CaAl hydrotalcite or hydroxyapatite decorated invasive plant ( Solidago canadensis )-derived biochar were synthesized by co-precipitation and high temperature pyrolysis method. The three composites and bare biochar were characterized by Scanning electron microscopy (SEM), X-ray spectroscopy (EDX), the Fourier transform infrared spectroscopy (FT-IR), X-ray diffractometer (XRD), and X-ray photoelectron spectroscopy (XPS) techniques, and employed to remove Eu(III) from wastewater under a series of environmental conditions. The results indicated that the Eu(III) adsorption on BC@LDH@HAP was higher than that on BC, BC@LDH, and BC@HAP, and belonged to multi-layer adsorption, which was different from the monolayer adsorption of biochar. The adsorption could be fitted best by Langmuir model and the maximum adsorption capacity of Eu(III) on BC@LDH@HAP was up to 714 mg/g at pH ~ 6. The characterization results suggested that this excellent adsorption of BC@LDH@HAP arose from the abundant P-, C-, O-containing functional groups rather than larger specific surface area. The spectra of XPS, FT-IR, and XRD uncovered that the adsorption mechanisms of Eu(III) on BC@LDH@HAP involved surface complexation, ion exchange, and precipitation. Moreover, the absorbed Eu(III) was formed into two precipitate induced by P-containing groups and carbonate groups. This research confirmed BC@LDH@HAP is a promising material for the removal of Eu(III) in wastewater.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Yuming Zhang,Junming Cao,Junzhi Li,Zeyu Yuan,Dongdong Li,Lili Wang,Wei Han
High-performance aqueous electrochemical energy storage technology has attracted extensive research interest due to its high safety and potential for commercialization. Herein, following the simultaneous doping-electrostatic synergistic assembly strategy, we synthesized the 2D/2D Co-doped NiMn-Layered double hydroxide (LDH)/V 2 CT x MXene (CNMV) composite materials that serve as advanced electrodes for aqueous energy storage devices, such as supercapacitors and zinc ion batteries (ZIBs). For supercapacitors, benefiting from the hetero ion doping effect, the as-assembled CNMV electrode exhibits a higher specific capacitance of 1005 F g −1 at a current density of 1 A g −1 . For the assembled asymmetric supercapacitor (ASC) devices, a high energy density of 30.16 Wh kg −1 at 0.7 kW kg −1 was achieved. Acting as the cathode for ZIBs, CNMV exhibits a high reversible capacity of 322.7 mA h g −1 at 0.2 A g −1 after 100 cycles, and a considerable energy density of 368.7 W h kg −1 at a power density of 246 W kg −1 . The battery-type transformation to the pseudocapacitance-type CNMV electrode for the supercapacitor was demonstrated by quantitative kinetic analysis, while phase transformation and Zn 2+ insertion/extraction for zinc ion storage mechanism were demonstrated by ex-situ XRD and XPS. This study provides a facile and effective approach for the design of high-performance MXene-based electrodes for aqueous electrochemical energy storage devices.
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CHEMICAL ENGINEERING JOURNAL
·
2019
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IF 8.355
Liying Wu,Junming Hong,Qian Zhang,Bor-Yann Chen,Ji Wang,Zhengyu Dong
This first-attempt study explored interactive function of oxygen vacancies, transition metals, and surface hydroxyl groups for persulfate (PS) activation, at different pH conditions. Oxygen vacancy-rich Fe 2 Co 1 -LDHs was fabricated via calcination in hydrogen atmosphere. The Fe 2 Co 1 -LDH possessed the maximal concentration of oxygen vacancies and abundant hydroxyl groups for effective functioning according to the characterization through X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR). The BPA-degrading efficiency in the LDHs/PS system indicated that Fe 2 Co 1 -LDH exhibited the most promising activated performance since oxygen vacancies could improve the catalytic efficiency to enhance electron transport phenomena between the Fe and Co. N 2 experiments proved that the presence of oxygen vacancies could promote the production of 1 O 2 and O 2 − . Phosphate and pH effect experiments showed the Fe 2 Co 1 -LDH/PS system stably maintained operation performance over a wide pH range for bisphenol A (BPA) removal with the effect of surface hydroxyl groups. Practical samples had little effect on the removal of BPA. According to the quenching experiments and EPR technology, SO 4 − was the main active radicals in acid and neutral conditions and apparently the OH played the crucial role at alkaline pHs. Two different major reaction routes at different pH levels in the Fe 2 Co 1 -LDH/PS system for mechanisms of BPA degradation were proposed herein. The Chemical intermediates of BPA degradation were identified by gas chromatography-mass spectrophotometry (GC–MS) analysis, and degradation pathways were proposed for system optimization.
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ANALYTICA CHIMICA ACTA
·
2018
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IF 5.123
Xuechao Xu,Xiaobo Zou,Shuwen Wu,Linjie Wang,Xiangheng Niu,Xin Li,Jianming Pan,Hongli Zhao,Minbo Lan
As pyrophosphate ion (PPi) and pyrophosphatase (PPase) play crucial roles in the pathological process of arthritis, determination of PPi and PPase in biological fluids turns to be of great importance for clinical diagnosis and therapy of arthritic diseases. In this work, we proposed a new fluorescent assay for PPi and PPase activity detection based on the competitive coordination chemistry of Fe 3+ between PPi and an in situ formed fluorescent polydopamine (PDA). FeCo layered double hydroxide (FeCo-LDH) was explored as a peroxidase mimic to facilitate the in situ formation of fluorescent PDA from dopamine mediated by low-concentration H 2 O 2 within 30 min; The formed fluorescent PDA could be significantly quenched by Fe 3+ through forming a PDA-Fe 3+ complex structure; When PPi existed, it coordinated Fe 3+ competitively against PDA and inhibited the fluorescence quenching of PDA by Fe 3+ ; When PPi was hydrolyzed under the catalysis of PPase, the Fe 3+ ion could quench the fluorescence of the formed PDA again. With these principles, our fluorescent assay was able to detect PPi and PPase activity specifically, providing detection limits down to 54 μM and 0.13 U/L, respectively. Furthermore, accurate determination of PPi and PPase activity in spiked human serum was also demonstrated using the developed assay.
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Inorganic Chemistry Frontiers
·
2024
·Vol. 12
·期 1
·179-190
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IF 6.1
Weiwei Han,Wenyi Wang,Jiahong Liao,Yi He,Xingwang Zhang,Chunlin Yu
Sustainable hydrogen production by electrocatalytic water splitting is a promising energy storage technology yet challenging due to the sluggish kinetics of the oxygen evolution reaction (OER). Rationally designed robust and high-efficiency non-noble metal electrocatalysts for large-current-density OER are highly desirable for industrial-grade hydrogen production. Herein, a unique hierarchical heterostructure electrocatalyst composed of FeCo layered double hydroxide nanosheets and a NiSe nanowire array grown on Ni foam (FeCo LDH/NiSe@NF) is demonstrated. The optimized FeCo LDH/NiSe@NF exhibits an excellent OER activity with low overpotentials of 230, 266 and 298 mV at current densities of 100, 500 and 1000 mA cm−2 in an alkaline solution. In particular, it can deliver 1000 mA cm−2 without much decay after the long-term stability test for 100 h. Both the experimental results and theoretical calculations reveal that reasonable construction of a hierarchical heterostructure, as well as the strong interaction at the heterointerface between NiSe and FeCo LDH can not only offer sufficient exposure of the surface active sites, better electrochemical conductivity and structural stability, but also effectively optimize electronic configurations and lower the reaction energy barriers, consequently facilitating the reaction kinetics especially in large-current-density alkaline water electrolysis. Moreover, a two-electrode electrolyzer using FeCo LDH/NiSe@NF and NiCoP/NiCoSx@NF as the anode and cathode only needs a cell voltage of 1.849 V to reach 1000 mA cm−2 in 30 wt% KOH solution at 80 °C. The high catalytic activity and long-term stability of the catalyst at large current densities have exceeded most electrocatalysts reported, highlighting its great potential in large-scale applications.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2024
·Vol. 39
·期 1
·e7942
·
IF 3.7
Di Su,Wen Xu,Dongbin Yang,Jiandu Lei,Jing Liu,Chunping Chen,Dermot O'Hare
As a renewable new material with high void ratio, large adsorption surface area, and high adsorption rate, biomass carbon (BC) is a promising adsorbent, which has received wide attention for the degradation of dyes. However, physical adsorption cannot completely remove dyes, and there is also the risk of secondary pollution. ZnAl-layered double hydroxide (ZnAl-LDH) is a semiconductor photocatalyst with abundant active sites and excellent degradation efficiency. In this paper, we have designed a ZnAl-layered double oxide@biomass carbon (ZnAl-LDO@BC) formed by in situ grown LDH on the waste poplar wood as a synergistic adsorption and photocatalytic system. BC as a support could enhance the dispersity of layered double oxide (LDO), whereas LDO could provide photodegradation function to BC. Our studies indicate that the prepared ZnAl-LDO@BC presents lower bandgap energy, higher surface area, and lower complexation efficiency of holes and electrons than delignified biomass (DB). As a result, ZnAl-LDO@BC increased the removal rate of malachite green (MG) to 85.8%, which is 3.5 times higher than DB. The maximum removal rate was close to 98%, and the removal capacity was 1954 mg g −1 under an initial concentration of 200 mg L −1 of MG dye, and the possible mechanism of MG degradation was also investigated. In this study, the conversion of agroforestry wastes into high-value materials applied to dye degradation provides a new pathway for the production of stable, sustainable, and superior photocatalytic material.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Xuyan Guo,Zhuangzhuang Xiong,Fuqiu Ma,Qizi Wu,Lixia Ying,Guixiang Wang
Ce-Co-Al Layered double hydroxides (LDH) coatings with WO 4 2− intercalation and 1H, 1H, 2H, 2H-Perfluorodecyltrimethoxysilane (PFDTMS) film was successfully prepared through in situ growth, ion exchange and self-assembly method. In this work, we designed a novel anti-corrosion system composed of a LDH coating as an anionic nano-container, an anionic corrosion inhibitor between layers and a superhydrophobic film that plays a barrier role. The morphology, structure and composition of different samples were characterized using SEM, EDX, XRD, FT-IR, and XPS. The performance of the samples was evaluated through electrochemical, contact angle, and wear behavior testing. The results revealed that PFDTMS-WO 4 2− -LDH exhibited superhydrophobic properties and excellent anti-corrosion performance compared to Al alloy, with a corrosion current density from 1.248 × 10 −5 A·cm −2 to 1.606 × 10 −10 A·cm −2 and a static contact angle from 76.3° to 152.8° Covering the Al alloy with Ce-Co-Al LDH resulted in the friction coefficient decreased from 0.7 to 0.2, demonstrating the superior tribological performance of LDH. It was confirmed that the main reason for the significant improvement of the long-term corrosion resistance of PFDTMS-WO 4 2− -LDH was the barrier function of the PFDTMS film and the corrosion inhibition effect of the Ce 3+ and WO 4 2− . This work is of great significance for the preparation of corrosion-resistant LDH and engineering an anti-corrosion system with the surface of the material.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yi Ma,Luming Li,Yong Zhang,Ning Jian,Huiyan Pan,Jie Deng,Junshan Li
Electrochemical upgrading methanol into value-added formate at the anode in alkaline media enables the boosting production of hydrogen fuel at the cathode with saved energy. To achieve such a cost-effective and efficient electrocatalytic process, herein this work presents a Mn-doped nickel iron layered double hydroxides supported on nickel foam, derived from a simple hydrothermal synthesis. This developed electrocatalyst could act as an efficient bifunctional electrocatalyst for methanol-to-formate with a high faradaic efficiency of nearly 100 %, and for hydrogen evolution reaction, at an external potential of 1.5 V versus reversible hydrogen electrode. Additionally, a current density of 131.1 mA cm −2 with a decay of merely 12.2 % over 120 h continuous long-term testing was generated in co-electrocatalysis of water/methanol solution. Further density functional theoretical calculations were used to unravel the methanol-to-formate reaction mechanism arising from the doping of Fe and/or Mn. This work offers a good example of co-electrocatalysis to produce formate and green hydrogen fuel using a bifunctional electrocatalyst.
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ENERGY & FUELS
·
2024
·
IF 5.2
Yuan-Ming Cao,Xue-Lei Duan,Miao Bian,Hou-Yu Wang,Yi-Wen Shen,Chong Gao,Chun-Gang Yuan
The immobilization of Hg0 and detoxication of Hg-containing composites are enormous challenges for Hg pollution control, which provide a high requirement for the design and synthesis of materials. Herein, a new composite with halloysite, selenium, and transition metals as raw materials (FeCo-LDH/HNTs@Se) for a Hg0 trap was designed by precipitation with ion exchange and an in situ selenization method. Intrinsic features such as high affinity, microwave permittivity (109–1012), large surface area, abundant pores, and many active components favored Hg0 removal and immobilization. The removal performance, flue gas tolerance, and synergistic effect of active components were improved greatly when microwave was added. The study indicated that (1) the Hg0 removal efficiency of the composite could reach 99.4%; (2) the composite had excellent tolerance to different industries’ flue gases. The electron exchange of Co(II)/Co(III) and Fe(II)/Fe(III) and the existence of Se and SeO2 were important for Hg0 immobilization. HgSe was the main adsorption product based on both X-ray photoelectron spectroscopy (XPS) and an online lab-built thermal decomposition system (TPD-AFS) analysis, which made the used-materials possess low mercury leaching content (0.09 mg·L–1) lower than the US EPA regulatory value (0.2 mg·L–1). This work provides a sound way for mercury control, which is significant for environmental protection.
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ENERGY & FUELS
·
2024
·
IF 5.2
Jiongyu Chen,Zhi Liu,Yuchen Liu,Zhen Cheng,Jingze Zhang,Qinghong Zhang,Yaogang Li,Chengyi Hou,Kerui Li,Hongzhi Wang
Efficient and affordable electrocatalysts are a crucial part of rechargeable zinc air batteries (ZAB) to address the problems caused by the sluggish activity of the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) on the cathode. Anchoring noble metals on transition-metal-based substances is a promising strategy to reinforce electrochemical activity and reduce the cost. Herein, we have developed a subsequent spontaneous-redox strategy to load Pt nanoparticles with 3.75% containing NiFe-LDH nanoflakes to boost the ORR activity. After that, NiFe-LDH@ Co9S8 is constructed as a rational design for bifunction catalysis. In the ORR process, the half-wave potential of the obtained catalyst, Pt-anchored NiFe-LDH@Co9S8, is 0.83 V vs RHE, showing better catalytic activity than Pt/C. In the OER process, the obtained catalyst exhibits a low overpotential of 280 mV, which is superior to that of RuO2. Notably, aqueous ZAB and quasi-solid-state ZAB achieve peak power densities of 164.3 and 78.4 mW cm–2, respectively. Furthermore, quasi-solid-state ZAB exhibits a long cycle lifespan for 240 cycles in 80 h, and a remarkable stability after bending for 50 cycles. This work paves the way for the design of the NiFe-LDH nanostructure by vacancy engineering.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yanmeng Cai,Guangyuan Zhao,Qing Yuan,Jinsheng Zhao
Layered double hydroxides (LDHs) have been recognized as prospective two-dimensional capacitive deionization (CDI) faradaic materials for Cl - capture, offering tunable interlayer distance, high anion exchange capacity, and reversible ion intercalation/deintercalation ability. However, the self-stacking tendency, poor electrical conductivity, and undesired stability of LDHs nanosheets severely impede ion migration and active sites accessibility, leading to unsatisfactory CDI performance. Herein, we present an elaborately designed three-dimensional sandwich structural composite N-doped porous carbon spheres/NiMn-layered double hydroxide/MXene (NPC/NiMn-LDH/MXene) to efficiently capture Cl - as the CDI anode. In this assembly, MXene not only ensures excellent electrical conductivity for rapid ion transfer but also serves as a robust substrate for the uniform dispersion of NiMn-LDH nanosheets. Moreover, NiMn-LDH effectively inhibits the agglomeration of MXene and provides substantial storage capacity for ion accommodation. The conductive intermedium NPC establishes interconnected conductive channels, enriching accessible charge transport pathways, resulting in an accelerated ion diffusion kinetics. Accordingly, the NPC/NiMn-LDH/MXene electrode demonstrated predominant specific capacitance (265 F g - 1 ), lower ion transfer resistance, and an optimized Cl - diffusion coefficient (7.95 × 10 -17 cm 2 s −1 ). In an asymmetrical CDI cell assembly, the NPC/NiMn-LDH/MXene//NPC cell delivered outstanding Cl - removal capacity (43.5 mg g −1 ), swift salt removal rate (12.5 mg g −1 min −1 ), efficient energy utilization (0.183 kWh kg −1 -NaCl), and remarkable cyclic adsorption/desorption stability (89.6 % retention rate). Additionally, density functional theory (DFT) calculations validated that the sandwich construction of NPC/NiMn-LDH/MXene facilitated interfacial charge transfer from NPC and MXene to NiMn-LDH, accelerated ion transfer rate, and reduced ion migration energy, resulting in accessible ion diffusion kinetics and smooth Cl - shuttle. This unique approach enriches ion transfer pathways by leveraging the distinctive structural characteristics of faradaic materials, providing valuable insights for further developments in CDI technology.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Shiwei Song,Yanhui Wang,Pengfei Tian,Jianbing Zang
The admire activity, selective and corrosion resistance electrocatalysts for oxygen evolution reaction (OER) are the bottleneck restricting seawater electrolysis owing to the side reactions of chloride ions (Cl − ). Herein, we developed a local amorphous S-modified NiFe-LDH ultrathin nanosheets with large spacing on NiFe foam (la-S-NiFe-LDH/NFF) in-situ via the fast H 2 O 2 assisted etching-anion regulation, resulting in a superior OER catalytic activity for seawater electrolysis. Benefitting from the local amorphous architecture induced by S, enhanced the metal–oxygen covalency, triggered lattice oxygen activity, and reduced the desorption energy of O 2 , the la-S-NiFe-LDH/NFF accelerated the OER progress via the lattice-oxygen-mediated (LOM) mechanism. Additionally, the preferential adsorbed OH – and reconstructed SO 4 2− cooperated to prevent the proximity and erosion of Cl − and enhanced the corrosion resistance for seawater electrolysis. The assembled electrolyzer of Pt/C || la-S-NiFe-LDH/NFF possessed an industrial level of 500 mA cm −2 at 1.83 V potential for seawater electrolysis, and sustained response for 100 h.
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