JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.6
Shizhe Liu,Yang Liu,Yi Ren,Menghao Kong,Tianfang Yang,Shilong Li,Pinghao Cui,Xinxin Jia,Liyuan Wang,Shuyan Gao
Dual-regulation via sp-N and Co nanoparticles optimizes the Co d-band center. • Operando SERS reveals rapid interfacial *OOH conversion for efficient 4e − ORR. • CoNP/Co@sp-N breaks the inherent ORR activity-stability trade-off effectively. • Catalyst yields 0.89 V E 1/2 and enables Zn-air batteries with >240 h stability. Single-atom catalysts have drawn massive interest for their ability to electrocatalyze the oxygen reduction reaction (ORR), primarily attributed to their ultimate atom economy and structurally distinct active centers. Nevertheless, simultaneously achieving robust durability and exceptional catalytic efficiency persists as a critical bottleneck. Herein we develop a graphyne-based composite material (CoNP/Co@sp-N) composite wherein sp-hybridized nitrogen (sp-N) anchored Co single atoms are synergistically coupled with adjacent cobalt nanoparticles. Density functional theory (DFT) reveals that while strong sp-N coordination provides robust atomic anchoring, the sp-N/nanoparticle electronic synergy precisely optimizes the Co d-band center to achieve near-ideal OOH binding, effectively decoupling the inherent ORR activity-stability trade-off. The unique coordination environment provides formidable orbital hybridization for unyielding atomic anchoring while the nanoparticle-induced electronic modulation optimizes the adsorption free energy of OOH intermediates. This synergistic integration bypasses the traditional compromise by simultaneously enhancing electrocatalytic efficiency and preserving operational stability. Notably, the CoNP/Co@sp-N composite delivers outstanding oxygen reduction performance, achieving a half-wave potential of 0.89 V, and exhibits zero efficiency loss following 5000 continuous cycles. Moreover, when incorporated into a functional zinc-air battery, this catalyst attained a peak power density of 187.33 mW cm −2 and exhibited remarkable cycling stability surpassing 240 h, thereby underscoring its significant potential for extensive energy conversion applications. A dual-regulation strategy breaks the oxygen reduction activity-stability trade-off via a graphyne-based CoNP/Co@sp-N composite. Strong sp-hybridized nitrogen coordination ensures robust atomic anchoring, while adjacent cobalt nanoparticles electronically modulate the Co single atoms to optimize OOH binding. This synergistic architecture drives highly efficient and durable O 2 -to-H 2 O conversion for advanced zinc-air batteries. Download: Download high-res image (173KB) Download: Download full-size image
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Catalysis Science & Technology
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2022
·Vol. 12
·期 10
·3209-3218
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IF 6.177
Meng Tian,Jing Qian,Jiawei Hou,Yadi Bai,Hai-Ying Jiang,Jingyun Ren
Free silver ions (Ag+) in the solution exhibit enhanced photocatalytic dechlorination processes of organic chloride, including 2-chlorophenol (2-CP), 2,4-dichlorophenol (2,4-DCP) and 2,4,6-trichlorophenol (2,4,6-TCP), over copper phenylacetylene (PhC2Cu) under visible light irradiation. The concentration of AgNO3 remarkably affects the dechlorination activity of PhC2Cu. With the optimal concentration of 2 mM AgNO3, PhC2Cu showed the best photocatalytic performance, and the dechlorination rate of PhC2Cu was 2.3-fold enhanced under visible light irradiation for 80 minutes. This deep mechanism study demonstrated that free Ag+ in the solution, but not the deposited Ag particles on the surface of PhC2Cu, plays the most imported role in promoting the photocatalytic dechlorination process by forming the insoluble salt of AgCl.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Tianyi Xu,Dongxu Jiao,Lei Zhang,Haiyan Zhang,Lirong Zheng,David J. Singh,Jingxiang Zhao,Weitao Zheng,Xiaoqiang Cui
Development of efficient electrocatalysts requires construction of catalytic surfaces with moderate H adsorption energy. Here, we address this challenge by Br-induced formation of P-poor defective nickel phosphide and show that the H adsorption energy can be optimized by regulating the vacancy concentration. We show that when such defective Ni 12 P 5−x Br x nanoparticles are distributed on the surface of Ni 2 P nanosheets (Ni 12 P 5−x Br x /Ni 2 P NS), excellent catalytic activity for water splitting is obtained in alkaline media. Density functional theory computations revealed that Br doping induce the formation of a P-poor nickel phosphide with vacancies, leading to an optimal H adsorption strength with a volcano-type relationship. This is the best reported for a non-precious metal phosphide at present: the overpotential for HER is 18 mV at 10 mA cm −2 and 155 mV for OER. This leads to an exceptionally low cell voltage requirement of only 1.44 V to drive overall water splitting in an alkaline electrolyzer.
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DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 42
·15422-15432
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IF 4.39
Dong Qiu,Chengli He,Yuxuan Lu,Qiaodan Li,Yang Chen,Xiaoli Cui
Photoelectrochemical water splitting is an excellent strategy for hydrogen generation and it is pivotal to the development of photoanodes with sufficient sunlight harvesting, rapid charge separation, and enhanced electron injection efficiency. In this work, we rationally constructed a γ-graphyne/TiO2 (GY/TiO2) p–n heterojunction in which p-type γ-graphyne nanosheets were distributed in the three-dimensional space surrounding TiO2 nanotube arrays. The GY/TiO2 photoanode achieves a photocurrent density of 0.75 mA cm−2 at 1.23 V (vs. RHE), 1.7 times that of bare TiO2, and extends the electron lifetime of TiO2 from 0.51 to 1.16 ms. The improvement arises from moderate γ-graphyne modification, contributing to broadened light absorption, the suppressed recombination of electron–hole pairs, an increase in charge transfer, and a higher injection efficiency of surface electrons. This work provides a reliable approach for the utilization and conversion of sustainable solar energy.
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FOOD CHEMISTRY
·
2022
·
IF 9.231
Jiannan Chen,Xiuhua Xia,Peizhen Li,Hang Yu,Yunfei Xie,Yahui Guo,Weirong Yao,He Qian,Yuliang Cheng
Natural N and S co-doped carbon dots (NSCDs) were synthesized via hydrothermal synthesis using food-derived crawfish shells as green precursors. The relationship between quantum yield (QY) and protein content of six crawfish shells treated with different alkalis was investigated. The synthesized NSCDs displayed a large QY of 18.57 %, which was higher than most of the chitin-derived CDs. Due to the oxidation of hydroxyl radicals, adding H 2 O 2 and horseradish peroxidase (HRP) quenched the fluorescence of NSCDs, resulting in a detection limit (LOD) of 1.25 μM for H 2 O 2 . The addition of pentachlorophenol (PCP) was supposed to consume part of the hydroxyl radicals and protect NSCDs from being oxidized. Accordingly, a facile and rapid “off–on” fluorescence sensor was developed to detect PCP with a LOD of 2.30 μM. Further, the method described was successfully used to detect PCP in three real samples.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Rui Hou,Siqi Zhang,Qianyi Huang,Lang Lin,Hengxiang Li,Jingxi Li,Shan Liu,Chengjun Sun,Xiangrong Xu
Ingestion is a major exposure route for hydrophobic organic pollutants in fish, but the microbial transformation and estrogenic modification of the novel plastic additives by the gut microbiota of fish remain obscure. Using an in vitro approach, we provide evidence that structure-related transformation of various plastic additives by the gastric and intestinal (GI) microbiota from crucian carp, with the degradation ratio of bisphenols and triphenyl phosphate faster than those of brominated compounds. The degradation kinetics for these pollutants could be limited by oxygen and cometabolic substrates (i.e., glucose). The fish GI microbiota could utilize the vast majority of carbon sources in a Biolog EcoPlate, suggesting their high metabolic potential and ability to transform various organic compounds. Unique microorganisms associated with transformation of the plastic additives including genera of Citrobacter, Klebsiella, and some unclassified genera in Enterobacteriaceae were identified by combining high-throughput genetic analyses and metagenomic analyses. Through identification of anaerobic transformation products by high-resolution mass spectrometry, alkyl-cleavage was found the common transformation mechanism, and hydrolysis was the major pathway for ester-containing pollutants. After anaerobic incubation, the estrogenic activities of triphenyl phosphate and bisphenols A, F, and AF declined, whereas that of bisphenol AP increased.
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ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Guiquan Liu,Guorong Wang,Zhiliang Jin
Porous carbon is an ingredient for energy transformation and collection systems in terms of electrochemistry. As a new member, graphdiyne (GDY) gradually began to be concerned because of its especially compositional and structural properties. Herein, a lamelliform GDY was successfully prepared by cross-coupling strategy under the catalysis of cuprous iodide. Thanks to the sp and sp 2 hybrid carbon networks, the obtained GDY nano-lamellas promote excellent performance in the electrode of supercapacitors with a gravimetric capacitance of 137.8 F g − 1 at a mass-specific current of 1 A g − 1 , and a relatively good rate performance of 81.28% when the mass-specific current reach to 20 A g − 1 . In addition, the capacitance of the GDY electrode barely decays during the 11,000 cycles of repeated testing. This enables the assembled symmetric supercapacitor provides a acceptable energy density of 6.11Wh kg −1 under a power density of 5500W kg −1 , and with an average decay of 0.5% per cycle at the end of 5000 cycles. The relatively good electrochemical stability of this GDY nano-lamellas material will open the further promotion of graphdiyne-based electrodes in the domain of supercapacitors.
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VACUUM
·
2023
·
IF 4
Zihan Wang,Xiaoqing Ma,Qiaodan Li,Xinyao Tian,Jilei Si,Mauricio A. Melo
Photoelectrochemical (PEC) water splitting is a viable method for converting renewable solar energy into storable chemical energy. Herein, the newly emerged two-dimensional sp- and sp 2 -carbon hybridized graphyne sheets were successfully coupled with thin film-like arrays of titanium dioxide nanorods , forming an efficient 2D-1D heterojunction . The microstructure and composition of obtained γ-graphyne/TiO 2 films were well characterized. And enhanced photoelectrochemical properties were demonstrated. The γ-graphyne/TiO 2 photoelectrode achieves a photocurrent density of 1.31 mA/cm 2 at 1.23 V ( vs. RHE), which is 1.7 times over that of pristine titanium dioxide. An improvement of photoconversion efficiency by 2.2 folds was observed. The high PEC activity of γ-graphyne/TiO 2 originates from band alignment and interfacial junction between π-conjugated graphyne sheets and TiO 2 nanostructure , greatly promoting charge transfer and diminishing defective excitation and recombination. By virtue of the γ-graphyne nanosheets , largely increased number of useful photons and catalytic active sites are triggered. This work provides a reference for the photoelectrochemical application of semiconductive γ-graphyne and a specific and proven method for the utilization of solar energy.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Huayan Fu,Ruiwen Luo,Panpan Liu,Shuning Yu,Qinglei Xing,Peng Bai,Xianghai Guo,Jiafei Lyu
Conquering the trade-off between selectivity and permeability is crucial for efficient ethanol dehydration. The sophisticated metal–organic frameworks (MOFs) have proven their potential as membrane fillers despite of the limited research on few frameworks. Herein, in order to achieve enhanced water permselectivity, hydrophilic zirconium-based NU-906 nanoparticles were incorporated into chitosan (CS) to fabricate NU-906/CS mixed matrix membranes (MMMs) for alcohol dehydration. The introduction of NU-906 brought excellent water affinity and structural stability to the hybrid membranes confirmed by the water contact angle and swelling resistance tests. Benefiting from the hydrophilicity and the ordered porosity of the incorporated NU-906, simultaneously enhanced water selectivity and permeability have been achieved on the hybrid membranes. The optimum membrane with 5.0 wt% NU-906 exhibited a high flux of 1086 g/(m 2 ·h) and an excellent separation factor of 2651 for 90 wt% ethanol dehydration at 76 ℃. This research has expanded the range of MOFs available for the fabrication of MMMs and provided new options for organic solvent pervaporation dehydration.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Tong Xin,Mingxuan Chen,Zewei Liu,Ruiwen Luo,Qinglei Xing,Peng Bai,Xianghai Guo,Jiafei Lyu
The past two decades have witnessed the potentials of metal–organic frameworks (MOFs) for the adsorptive separation of difficult mixtures due to their designable porosity and significant surface area. In this work, two Zr 6 -based metal–organic framework materials with different pore sizes, NU-906 and NU-1008, were synthesized and evaluated as adsorbents for fructose/glucose separation, which is very important for sustainable biomass utilization. The two materials were characterized and studied, including the kinetics, isotherms, and thermodynamics by batch adsorption experiments, which can be well described by pseudo-second-order kinetics and Langmuir model (NU-906), Freundlich model (NU-1008), and the adsorption mechanism is described in terms of pore exclusion. The experimental results showed that NU-906 exhibited record-breaking adsorption selectivity towards fructose, whose static selectivity factor was up to 13.7. The NU-906 material with expanded particle size was further studied as filling of the chromatographic column for dynamic adsorption, and the dynamic selectivity factor was about 4.0, which was much higher than the column selectivity factor (∼2.5) used in the industry at present. In addition, three adsorption/regeneration experiments demonstrated its reusability.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Fan Li,Lei Lei,Yuxi Zhou,Xiaochen Wang,Yindan Zhang,Jianghuan Hua,Jian Han,Lihua Yang,Bingsheng Zhou
The novel brominated flame retardants (NBFRs) have received wide concerns due to their ubiquitous occurrence in the environment and their potential risks to ecosystems and human health. However, the toxicity data of NBFRs are still lacking, especially their toxicity comparison data, and toxicity predictions for untested NBFRs are extremely limited. In this study, eight commonly used NBFRs and decabromodiphenyl ether (BDE209) were selected to compare their toxicity at concentrations between 0.03 and 3.69 μM, by exposing zebrafish embryos until 120 h post-fertilization (hpf) and evaluating 18 toxicity indicators including basic development indicators and a series of behavioral indicators. The toxicity potency of the tested compounds ranked by the total number of significantly affected endpoints were pentabromobenzene (PBB) ≈ 2,4,6-tribromophenol (TBP) > BDE209 ≈ bis(2-ethylhexyl) tetrabromophthalate (TBPH) > pentabromotoluene (PBT) ≈ 2-ethylhexyl-2,3,4,5-tetrabromobenzoate (EHTBB) > 1,2-bis(2,4,6-tribromophenoxy)ethane (BTBPE) > hexabromobenzene (HBB) > decabromodiphenyl ethane (DBDPE). Almost all the tested compounds affected the locomotor behavior of zebrafish larvae, suggesting that the refined behavioral indicators were sensitive endpoints. Furthermore, the quantitative structure-activity relationship (QSAR) model we developed suggested that molecular surface area (MSA) might be the critical factor for determining the developmental neurotoxicity of NBFRs to zebrafish larvae, except for congeners with larger molecules (e.g. DBDPE, BTBPE). These findings would contribute to elucidating the toxicity differences among various NBFRs and provide important references for their toxicity prediction.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Meijuan Ding,Mei Li,Yijun Wang,Ziyu Li
Metal oxides have excellent photocatalytic properties. In this work, LDHs are used as precursors to prepare metal oxides (Cu 0.04 Zn 0.47 Co 2.49 O 4 ). Synthesis of graphdiyne (GDY) by mechanochemical method using calcium carbide as raw material. It is complexed with Cu 0.04 Zn 0.47 Co 2.49 O 4 to explore the hydrogen evolution performance of the composite catalyst CZC (Cu 0.04 Zn 0.47 Co 2.49 O 4 )/G (GDY) in water splitting under visible light and its possible hydrogen evolution mechanism. The results show that the composite catalyst CZC/G-11 has good hydrogen evolution activity, and its photocatalytic hydrogen evolution activity could reach up to 17.7 μmol h −1 at pH = 9. The four hydrogen evolution cycle stability tests show that CZC/G-11 maintains a relatively smooth level of hydrogen evolution. The photoelectrochemical and fluorescence test results show that the incorporation of GDY can effectively improve the charge separation efficiency of the composite catalyst CZC/G-11. Both CZC and GDY are n-type semiconductors, as shown by the Mott-Schottky test results. The catalysts are also tested by UPS and the energy band structure is analyzed, with conduction band values of −0.54 V and −0.58 V and valence band values of 1.41 V and 0.83 V for CZC and GDY, respectively. Combined with the electron transfer direction of each catalyst, the possible mechanism of photocatalytic hydrogen evolution between CZC and GDY is analyzed, and it is speculated that Z-scheme heterojunction is formed between CZC and GDY to promote the hydrogen evolution reaction.
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