CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Yutong Luo,Jiaheng Qin,Guangxue Yang,Sha Luo,Ziming Zhao,Ming Chen,Jiantai Ma
The rational design and fabrication of distinctive coordination sites is an attractive and challenging approach to develop electrocatalysts with superior activity toward oxygen evolution reaction (OER). Constructing N-doped carbon shells coordinated with transitional metal composites can greatly enhance the OER activity of electrocatalysts. Herein, a facile electrochemical-pyrolysis strategy is applied to synthesize NiS/C 3 N 4 composite with N-Ni-S coordination sites by in-situ crystallization on copper foam (CF). A detailed characterization, especially synchrotron-based X-ray absorption fine structure (XAFS) clearly unravels the N-Ni-S coordination mode is successfully formed. As a result, NiS/C 3 N 4 presents excellent OER performance with a low overpotential of 334 mV at a current density of 10 mA cm −2 , a Tafel slope of 45 mV dec −1 , and robust electrochemical stability for 50 h in basic media, outperforming some recently reported conventional transitional metal electrocatalysts. The outstanding electrocatalytic performance of NiS/C 3 N 4 mainly originates from the N-Ni-S coordination sites, which can provide abundant catalytic active sites, facilitate charge transfer, and enhance electronic conductivity. Furthermore, by tuning the two important experimental parameters of electrodeposition potential and electropolymerization time, the relationship between morphology and electrocatalytic performance of catalysts is deeply explored. This work demonstrates the validity of improving electrocatalytic performance by elaborately tailoring the coordination sites, thereby opening up an applicable and inspiring avenue forward in the design of advanced electrocatalysts for water splitting.
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APPLIED SURFACE SCIENCE
·
2020
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IF 6.182
Jinge Du,Zhe Xu,Hui Li,Haijun Yang,Shengjun Xu,Jun Wang,Yanan Jia,Shuanglong Ma,Sihui Zhan
A novel Z-scheme Ag 3 PO 4 /g-C 3 N 4 heterostructures was constructed successfully for Escherichia coli inactivation and organic pollutants degradation under visible light irradiation. The Ag 3 PO 4 (8)/g-C 3 N 4 possessed the highest photocatalytic effect with more than 7 log of live Escherichia coli ( E. coli ) totally inactivated within 75 min and complete BPA degradation within 180 min. By mimicking the components of natural water individually, humic acid (HA) and inorganic anion were found to deeply affected the photocatalytic disinfection activity. Moreover, the Ag 3 PO 4 (8)/g-C 3 N 4 revealed significantly boosted visible-light-driven photocatalytic performance for ciprofloxacin and sulfadiazine degradation. The satisfying degradation effects of bisphenol A in nature waters were also obtained. The improved photocatalytic efficiency of Ag 3 PO 4 /g-C 3 N 4 may be attributed to the formation of Z-scheme heterostructure structure and matching valence band and conduction band, resulting in rapid separation of photo-induced carrier, enhanced electronic transport capacity and prolonged carrier lifetime. The possible mechanism was studied using radical quenching tests and electron spin resonance, suggesting that the hole, electron and hydroxyl radical were the paramount active species during Escherichia coli disinfection. This work pioneers a novel strategy for upgrading the photocatalytic disinfection and degradation capacities of g-C 3 N 4 based catalysts.
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高影响因子
ACS Applied Energy Materials
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2021
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IF 6.024
Yiwen Hong,Jingxia Yang,WonMook Choi,Jinjie Wang,Jingli Xu
For increasing the specific capacitance of supercapacitors, boron-doped g-C3N4 quantum dots (B-CNQDs) were synthesized by KOH cutting and further adsorbed on the surface of Ni(OH)2 nanoflowers (B-CNQDx-Ni) by a mild impregnation method via electrostatic force. The B-CNQDx-Ni nanocomposites exhibit an increased surface area and reduced band gap energy compared with pure Ni(OH)2, which result in a larger contact area between the electrode and the electrolyte and enhanced charge-transfer kinetics. The best B-CNQDx-Ni sample has an excellent specific capacitance of 1700 F/g at 1.5 A/g, low impedance at the alkaline conduction of 7.421 Ω, and a high stability cycling performance of 82% capacity retention after 5000 cycles, suggesting that B-CNQDx-Ni is a type of suitable electrode material used in supercapacitors.
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
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2021
·
IF 3.927
Hongbing Song,Lei Liu,Haozhong Wang,Bingxiao Feng,Meng Xiao,Yubao Tang,Xiaofei Qu,Hengjun Gai,Tingting Huang
The development of a photocatalyst with high activity, large specific surface area and precise band gap adjustment is the focus of the field of photocatalysis in realizing energy conversion and improving environmental issues. In this paper, a simple synthesis process for co-doping of KCl and NH 4 Cl to precisely adjust the band gap of g-C 3 N 4 was developed. Various characterization results show that doping with KCl and NH 4 Cl can reduce the band gap of the carbon nitride , increase its visible light absorption, improve its carrier separation efficiency, thus showing good photocatalytic activity . Cl and K enter the g-C 3 N 4 layers via intercalation and form a dual-element charge transport channel between these layers, thereby facilitating the transport of electrons. The introduction of NH 4 Cl increases the specific surface area of the composite, thus providing abundant adsorption and reaction sites. The co-loaded photocatalyst CN-NH 4 Cl-0.05KCl was used to degrade rhodamine B (RhB) and tetracycline (TC) and showed excellent photocatalytic activity. A possible mechanism of photocatalytic degradation is proposed based on the analytic results.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
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IF 3.99
Haiping Liu,Jing Liang,Shuai Fu,Li Li,Jiehu Cui,Penghui Gao,Fengying Zhao,Jianguo Zhou
Exploiting metal-free cocatalysts is of huge interest for photocatalytic technology in environmental wastewater remediation and water splitting fields. The N doped carbon quantum dots (NCDs) modified defect-rich g-C 3 N 4 (DCN) was prepared through impregnation method. The structural, optical and electronic properties of NCDs/DCN were systematically investigated. The NCDs/DCN with outstanding visible light absorption, narrowed gap and electron transfer ability were conducive to combined pollutions photocatalytic removal and simultaneous H 2 production and rhodamine B (RhB) degradation. The resulting NCDs/DCN performed much higher removal efficiency in different combined pollutions systems containing OFL/Cr (VI), BPA/Cr (VI) and CIP/Cr (VI) than in single system owing to the synergistic effect between organic pollution oxidation and Cr (VI) reduction. The free-radical quenching experiments, spectral technology and electron spin resonance (ESR) confirmed that Cr(VI) can be reduced by the conduction band (CB) electrons, and the h + and O 2 − radicals dominated OFL degradation. The optimized NCDs/DCN displayed excellent simultaneously photocatalytic H 2 production activity and RhB degradation with the H 2 evolution rate of 3.68 μmol‧h −1 ‧g −1 and 100% RhB removal efficiency. The photocatalytic activity of simultaneous combined pollutions removal and synergistic H 2 generation and RHB degradation provides a promising strategy for real wastewater remediation applications and energy utilization.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2020
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IF 6.551
Zhiwei Zhao,Wei Zhang,Wen Liu,Yunyi Li,Jiangyu Ye,Jialiang Liang,Meiping Tong
In this work, a novel strategy for building single-atom silver-induced amorphous graphitic carbon nitride (g-C 3 N 4 ) with a hollow tubular morphology is developed. By forming a tubular supramolecular gel, silver is successfully isolated by the nitrogen atoms in both melamine and nitrate anions, impeding agglomeration in the subsequent thermal polymerization. The high density of single-atom-dispersed silver (atomic ratio up to 11.6%) selectively breaks the hydrogen bonds in layered g-C 3 N 4 , leading to a fully amorphous structure. Silver-induced full amorphization not only enhances the visible light absorption of g-C 3 N 4 but also accelerates charge transfer, endowing the as-prepared photocatalyst having the optimal silver content with 52 times higher surface area specific naproxen (NPX) removal activity than pure g-C 3 N 4 . Both density functional theory (DFT) calculations and steric effects are applied to explain the degradation pathway of NPX. The toxicity of NPX is reduced by sufficient irradiation. This work provides useful insights into the design and morphology control of single metal ion-dispersed g-C 3 N 4 for environmental applications.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Lei Chen,Jin-Tao Ren,Zhong-Yong Yuan
The modification of electronic structure in heterogeneous catalysts has been particularly proven as one of efficient approaches for enhancing the catalytic performances in redox. Herein, phosphorus-doped g-C 3 N 4 nanosheets with atomically dispersed V-based nanocomposites (V/P-CN) were fabricated through a facile organophosphonic acid-modified co-condensation route. The use of organophosphonic acid not only achieves the in-situ P-doping but also tailors the texture of the synthesized V/P-CN, leading to narrow band gap, electron-enriched structure, nanosheet morphology, abundant mesh-like pores and enlarged surface area. Series of physicochemical and electrochemical characterizations indicate the enhanced electron transfer from the P-doped g-C 3 N 4 to V-based nanocomposites. The heterojunction-induced electron–enriched structure of V-based nanocomposites in V/P-CN endows with the impressive intrinsic oxidative desulfurization activities. Radical scavenger experiment further suggests the significant electron interaction in the heterojunction catalysts favors the enriched electron dispersion around V-based active species and employs as rate-determining step for oxidative desulfurization. This work offers a facile but economic and powerful method to modulate the structure of the heterojunction catalysts for green catalysis, especially redox reactions.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
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IF 3.99
Xuecheng Liu,Lin Liu,Zurun Yao,Zhehan Yang,Hui Xu
The nitrogen-rich ZnO/g-C 3 N 4 composites were prepared and exhibited excellent photocatalytic performance for hydrogen evolution and NO photo-oxidation under visible-light illumination. The obtained nitrogen-rich ZnO/g-C 3 N 4 composite has efficient visible-light utilization and effective separation of photogenerated electron-hole pairs. Experimental data verifies that the photocatalytic activity of ZnO/g-C 3 N 4 composite could be improved by N dopant. NZnOCN1 composite exhibits the highest photocatalytic activity for H 2 evolution and NO removal. The results show that the possible mechanism of the photocatalytic H 2 evolution reaction is the type II mechanism, while the Z-scheme mechanism of nitrogen-rich ZnO/g-C 3 N 4 composite is conducive to NO photo-oxidation.
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MICROCHIMICA ACTA
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2019
·Vol. 186
·期 11
·1-8
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IF 5.479
Duan Wei,Yan Pengcheng,Dong Jintao,Chen Yun,He Xiaoyang,Chen Jianping,Qian Junchao,Xu Li,Li Henan
A self-powered photoelectrochemical (PEC) aptamer probe is presented for the determination of oxytetracycline (OTC). The assay is based on the use of g-C 3 N 4 and NiO nanocrystals (NCs) which form a heterojunction. The latter was prepared by two-step hydrothermal pyrolysis by using the ionic liquid 1-hydroxyethyl-3-methylimidazole chloride which functions as a morphological template to form NiO NCs. The heterojunction exhibits much better electronic conductivity, wider absorption range, higher electron-hole-separation productivity, and stronger photocurrent compared to plain g-C 3 N 4 . The heterojunction was adopted to construct a self-powered PEC aptamer probe for OTC detection. An OTC-binding aptamer was immobilized on the heterojunction and the probe was constructed. The aptamer on the probe binding with OTC can form steric hindrance for transmitting of electrons and cause the PEC signal change depending on the OTC concentration. The photocurrent decreases with increasing OTC concentration in the 0.01 to 100 nM concentration range and its detection limit is 4 pM (at S/ N = 3).
Schematic representation of a self-powered photochemical aptamer probe. The probe performs enhanced ability for oxytetracycline (OTC) determination due to the formation of NiO nanocrystals/g-C 3 N 4 (NiO NCs/g-C 3 N 4 ) heterojunction and the specification recognition of the aptamer.
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JOURNAL OF HAZARDOUS MATERIALS
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2019
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IF 7.65
Yanping Hou,Guiyun Yuan,Shuangfei Wang,Zebin Yu,Shanming Qin,Lingli Tu,Yimin Yan,Xixi Chen,Hongxiang Zhu,Yankui Tang
In this study, a self-biased bio-photoelectrochemical system (SB-BPES) was constructed using a bioanode and the g-C 3 N 4 /CdS heterojunction photocathode for nitrofurazone (NFZ) degradation under solar irradiation. The physio-chemical properties and optical performance of photocatalysts were characterized, and photo-electrochemical properties of various photocathodes were analyzed. Results showed that g-C 3 N 4 /CdS exhibited the broadest visible light absorption range (to 594 nm) and the most efficient e − -h + separation; and its corresponding photocathode showed the highest photocurrent (9.8 μA), and the lowest charge transfer resistance (5.43 ☓ 10 3 Ω). In the solar-illuminated SB-BPES with g-C 3 N 4 /CdS photocathode, about 80% of NFZ removal rate was achieved within 10 h. More importantly, TOC removal of 62.6% was achieved in 24 h, which was 1.8 times of that from the open circuit SB-BPES, and 4.3 folds of that from microbial degradation; also, about 1.5 times of those from SB-BPES with g-C 3 N 4 and CdS photocathodes. Besides, reproducible current generations (∼1.0 mA) were produced. These verified that it was a self-sustained system for spontaneously pollutants degradation and electricity generation. Moreover, possible degradation mechanism and pathways were proposed according to the identified intermediates. This study provides inspiration for synchronic improving refractory organics degradation and net energy recovery.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2019
·Vol. 55
·期 10
·4358-4371
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IF 3.442
Zhu Zhi,Ma Changchang,Yu Kesheng,Lu Ziyang,Liu Zhi,Yan Yongsheng,Tang Xu,Huo Pengwei
It is still a challenging work to realize the universality of photocatalytic materials for unselectively removing environmental pollutants in water. Here, a ternary magnetism CoFe 2 O 4 /g-C 3 N 4 /HNTs heterojunction photocatalyst is firstly prepared, and the morphology, crystalline property, surface area, and magnetic recycling capability of the photocatalyst were investigated. The CoFe 2 O 4 /g-C 3 N 4 /HNTs shows a superior degradation efficiency for degrading 2-mercaptobenzothiazole (MBT) than that of pure g-C 3 N 4 . The high degradation performance that derives from the hollow structure of halloysite nanotubes (HNTs) can inhibit stacking of g-C 3 N 4 , which results in a larger specific surface area and more abundant reaction sites. Meanwhile, the heterojunction structure between g-C 3 N 4 and CoFe 2 O 4 improved the separation efficiency of charge carriers. In addition, the intermediate products, degradation pathway, and reaction mechanism of representative MBT pollutant over the CoFe 2 O 4 /g-C 3 N 4 /HNTs photocatalyst are revealed in depth. This work makes an important development.
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Nanoscale Advances
·
2019
·Vol. 2
·期 1
·274-285
·
IF 0
Qun Wang,Sicao Yu,Wei Qin,Xiaohong Wu
Two phase photocatalysts can be intergrown with each other, resulting in superior photocatalytic properties. Herein, methylamine lead bromide (MAPbBr3) wrapped/entrapped protonated graphitic carbon nitride (p-g-C3N4) intergrowth microcrystals were fabricated by mixing a pervoskite precursor with p-g-C3N4 colloidal sol. A highly stable isopropanol (IPA) solvent based photocatalytic system for dye degradation was demonstrated. The composite with an optimal p-g-C3N4 mass percentage of 3.3 wt% (denoted as MAPbBr3/p-g-C3N4-1.0 mg) exhibited the highest photocatalytic degradation of malachite green (99.8%) within 10 min under visible light, which was 5.3-fold and 16-fold greater than that exhibited by its constituents separately. The strong chemical interaction and fundamental photophysical processes in MAPbBr3/p-g-C3N4 were systematically evaluated by spectroscopic and electrochemical techniques, confirming the effective separation of photogenerated electron–hole pairs and faster interfacial charge transfer behavior. Furthermore, active superoxide radicals (O2˙−) played a vital role in the catalytic reaction, because of the significant photoinduced electron transfer rate (ket) in the inverted type-I core/shell MAPbBr3/p-g-C3N4 band configuration structure. In addition, MAPbBr3/p-g-C3N4 has good cycling stability for 10 cycles and versatility for other cationic (RhB) and anionic (MO) dye pollutants, indicating the great potential for solar energy conversion into chemical energy.
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