Catalysis Science & Technology
·
2023
·Vol. 13
·期 3
·898-909
·
IF 5
Haohui Gu,Feng Liang,Xiaohan Wang,Shuaibing Wu,Gongye Lv,Haijun Zhang,Shaowei Zhang,Lilin Lu,Zhijun Dong
The design of heterojunction photocatalysts is regarded as a very effective method to solve the high recombination rate of photogenerated charge carriers for CO2 photoreduction into hydrocarbons, and interface engineering is urgently required to achieve high efficiency. Herein, graphitic carbon nitride (g-C3N4, CN) was uniformly grown on the surface of nitrogen-doped rutile TiO2 (NT) nanorods by in situ deposition, and a NT@CN core/shell step-scheme (S-scheme) heterojunction system composed of NT nanorods and g-C3N4 was synthesised. The as-synthesised heterojunction containing 55 wt% g-C3N4 delivered the highest CO2 photoreduction activity (33.35 μmol g−1 for CO) without additional cocatalysts or external sacrificial agents, which was 7.1 times higher than that of bare NT nanorods. This improved CO2 reduction activity was attributable to the large surface area and impactful S-scheme heterostructure, which imparted the catalyst with sufficient visible-light harvesting ability, promoted the segregation and transformation of the photoinduced charge pairs, and enhanced the redox ability of the carriers. Concurrently, the NT@CN photocatalyst exhibited excellent reusability and stability. This work offers a new basis for designing and preparing rutile TiO2-based S-scheme heterojunctions with enhanced CO2 reduction performance.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Sheng-Zhe Zhao,Ran Lu,Yi Yang,Yun Lu,Raul D. Rodriguez,Jin-Ju Chen
Photocatalysis has a broad prospect for generating H 2 and reactive oxygen species . In this study, porous nanotubular g-C 3 N 4 /TiO 2 photocatalysts were obtained via electrospinning combined with an innovative vapor deposition approach. The waste foam was used as the precursor material for TiO 2 nanotubes , reducing production cost and benefiting resource recovery. The modification of g-C 3 N 4 onto TiO 2 nanotubes provided extensive active sites with an increased specific surface area and produced the heterojunction to improve charge separation. The g-C 3 N 4 /TiO 2 nanotubes displayed remarkable photocatalytic effects in the degradation of organic dye with a removal efficiency of 93.4% and H 2 evolution reaction performing at 4122 μmol·g −1 ·h −1 under simulated sunlight. Photocatalytic activation product analyses and density functional theory (DFT) calculations demonstrated a possible photogenerated carriers transfer pathway. This work provides a way to prepare multifunctional porous nanotubes using a facile synthesis method from abandoned resources with implications for environmental remediation and hydrogen generation.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Rongping Xu,Jinlong Li,Guozhe Sui,Yan Zhuang,Dongxuan Guo,Ze Luo,Shuang Liang,Hong Yao,Chao Wang
The construction of heterojunctions is considered as an effective strategy to boost catalytic degradation activity of photo-Fenton catalyst. Herein, a series of CdS@CuS/g-C 3 N 4 (CC-x/CN) heterojunctions have been successfully prepared by hydrothermal and cation exchange process, which have been applied for the removal of methyl orange (MO) via photo-Fenton process. The results demonstrate that the exchange of Cu 2+ for Cd 2+ on g-C 3 N 4 could inhibit the aggregation of CdS@CuS and increase the light absorption range and the active sites. Under visible light illumination, CC-10/CN (molar ratio of CuS to CdS is 10%) exhibits the optimal photo-Fenton-like catalytic performance with the degradation efficiency of 96% towards MO (40 mg L −1 ) and the total organic carbon removal rate of 75% within 35 min illumination. The apparent reaction rate constant of CC-10/CN (0.088 min −1 ) is approximately 22 and 6.29 times higher than those of pure g-C 3 N 4 and CdS@CuS (molar ratio of CuS to CdS is 10%), respectively. The enhanced photo-Fenton catalytic activity of CC-x/CN is mainly ascribed to the formation of the photo-Fenton effect between CC-10 and g-C 3 N 4 , which promotes the conversion and recycling of Cu 2+ and Cu + . Meanwhile, the successful formation of the heterojunctions reduces the recombination rate of carriers. In addition, the cycling experiments demonstrate that CC-10/CN possesses favorable stability and recoverability. Overall, the well-designed CC-x/CN heterojunctions reveal desirable potential application in the effective treatment of sewage via photo-Fenton process.
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CARBON
·
2023
·
IF 10.9
Hao Wang,Jiangwen Liao,Jiajun Zhong,Yunpeng Liu,Lei Yao,Lixiong Qian,Yuecheng Lai,Xin Wang,Yikun Li,Jianxin Song,Xueqing Xing,Guang Mo,Zhongjun Chen,Zhonghua Wu
In this paper, the unclear Ni atom coordination structure evolution in one-pot pyrolysis method synthesizing Ni single atom catalyst using graphitic carbon nitride as support (Ni-g-C 3 N 4 ) was deeply discussed. In-situ X-ray absorption fine structure spectra and other assisted methods were used to characterize the structural evolution. The results demonstrate that the pyrolysis process can be divided into three stages. In the first stage from room temperature to 183 °C (Stage I), the NiCl 2 ⋅6H 2 O was mixed with the supporting material (dicyandiamide) to form the precursor with Ni-(H 2 O) 6 octahedral coordination configuration. In the second stage from 183 to 350 °C (Stage II), the H 2 O molecules have been removed and the supporting material was converted to melamine. The melamine molecules were polycondensed to melem during 308–350 °C. The intermediates labeled Ni-melamine and Ni-melem was formed with Ni-N 4 planar quadrilateral coordination configuration. In the third stage from 350 to 600 °C (Stage III ), the supporting material (melem) was gradually converted to g-C 3 N 4 , and the Ni-N 4 coordination configurations were replaced by Ni-N 6 planar hexagon coordination configuration one by one. The three Ni coordination configurations were further confirmed by Reverse Monte Carlo simulations and ab initio calculations .
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Materials Today Nano
·
2023
·
IF 10.3
Jing Yan,Faguang Ma,Yilin Wu
Molecularly imprinted membranes have superior selective separation capacity, rebinding capacity, and flux due to their microporous substrates and tightly packed molecularly imprinted polymers . In current study, artemisinin (Ars), the most effective antimalarial drug , is used as template molecule. The permeation-selectivity wooden membranes based on Ars-imprinted nanocages designed by metal organic framework@carbon nitride self-assembly process (MDWMs) has been successfully prepared: (i) based on three-dimensional mesoporous basswood membranes, dopamine-based auto-polymerization process was developed on basswood to for harvest the first layer imprinting and secondary reaction platform. (ii) The two-dimensional sheet carbon nitride modified by metal-organic framework is stably loaded on the surface of the polydopamine-modified basswood membrane, providing a rich irregular point array structure for the formation of recognition sites. Based on elaborate designs and optimizations, selectivity , rebinding capabilities, and flux are enhanced on the developed MDWMs ( β Are/Ars = 6.49, β Aru/Ars = 4.22, β DH-Ars/Ars = 7.42), and high regeneration rate (>94% after 10 cycles) indicates that MDWMs have superior selectivity and stability. The MDWMs and preparation strategies developed here will provide a completely new design methodology for subsequent selective separation of Ars.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 30
·10515-10521
·
IF 4
Yun Wu,Rui Yao,Qiang Zhao,Jinping Li,Guang Liu
The electrolysis of water, particularly proton exchange membrane (PEM) water electrolysis, holds great promise for hydrogen production in industry. However, the catalyst used in this process is prone to dissolution in acidic environments, making it imperative to develop cost-effective, highly efficient, and acid-stable electrocatalytic materials to overcome this challenge and enable large-scale application of PEM water electrolysis technology. Herein, we prepared ruthenium oxide (RuO2)/graphitic carbon nitride (g-C3N4) composites (RuO2/C3N4) via a combination of sol–gel and annealing methods. The g-C3N4 provides a large surface area, while RuO2 is uniformly deposited on the g-C3N4 surface. The interaction between g-C3N4 and RuO2 stabilizes the RuO2 nanoparticles and enhances long-term water oxidation stability. This unique structure and the combined advantages of RuO2 and g-C3N4 yield exceptional electrocatalytic activity toward both the oxygen evolution reaction (OER, 240 mV@10 mA cm−2) and the hydrogen evolution reaction (HER, 109 mV@10 mA cm−2), with excellent durability (over 28 h), and a cell voltage of 1.607 V at 10 mA cm−2 when used in an RuO2/C3N4||RuO2/C3N4 electrolyzer. This study highlights the efficacy of the g-C3N4 support method in designing highly stable Ru-based OER electrocatalysts for efficient acidic water splitting.
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PubMed
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Advanced Energy and Sustainability Research
·
2023
·Vol. 4
·期 10
·2300072
·
IF 5.8
Haohui Huang,Xingqiang Liu,Feng Li,Qingyun He,Chengfa Tao,Longfu Wei,Changlin Yu,Hongbing Ji
Herein, well-crystallized ZnTiO 3 particles are first prepared by hydrothermal method. A series of S-scheme heterojunction photocatalysts of ZnTiO 3 /g-C 3 N 4 (referred to as ZTO/CN) with different mass ratios are synthesized by successfully doping ZnTiO 3 in g-C 3 N 4 precursors and loading ZnTiO 3 onto g-C 3 N 4 nanosheets by calcination. It is clearly found that the ZnTiO 3 particles are successfully loaded on g-C 3 N 4 nanosheets by the X-ray diffractometer, energy-dispersive X-ray spectra, and high-resolution transmission electron microscopy images. Moreover, the specific surface area of 3.0% ZTO/CN is higher than that of pure g-C 3 N 4 . Using triethanolamine as the hole sacrificial agent, the highest CO and H 2 yields are achieved in the 3.0% ZTO/CN composite catalyst under the xenon lamp irradiation for 1 h. The generation rates of CO and H 2 reach 15.19 and 5.77 μmol g −1 h −1 , respectively, which are 2.9 and 4.1 times higher than that of pure g-C 3 N 4 . The CO and H 2 yields of the ZTO/CN composite catalyst show a trend of increasing and then decreasing with the increasing of ZnTiO 3 content, which is due to the fact that excess ZnTiO 3 can lead to a reduction of the effective heterojunction interface between ZnTiO 3 and g-C 3 N 4 , decreasing the transfer and separation efficiency of photogenerated electrons and holes and thus reducing the photocatalytic activity.
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Catalysts
·
2022
·Vol. 12
·期 9
·1043
·
IF 4.501
Shuang Tang,Yang-Sen Xu,Wei-De Zhang
Molecular skeleton modification has become a recognized method that can effectively improve the photocatalytic performance of g-C3N4because it not only effectively promotes charge separation, but also tunes the conjugated system of g-C3N4to make it more conducive to photocatalytic reaction. Herein, thiophene-amide embedded g-C3N4(TA-CN-x) was successfully prepared by simple one-step thermal polycondensation using urea as a precursor and ethyl-2-amino-4-phenylthiophene-3-carboxylate (EAPC) as an additive. After embedding with thiophene-amide, the induction and delocalization effects are formed in TA-CN-x, which significantly improves the migration efficiency of photogenerated charge carriers. Meanwhile, the conjugate structure is changed due to structural modification, resulting in significant enhancement of visible light absorption compared to the pure g-C3N4(CN). Specifically, the optimized photocatalytic H2evolution rate of TA-CN-2 reaches 245.4 μmol·h−1, which is 8.4 times that of CN (with Pt nanoparticles as a co-catalyst), and the apparent quantum efficiency (AQY) at 450 nm is 13.6%. This work opens up a new modification process for fully tapping the photocatalytic hydrogen absorption potential of g-C3N4-based materials.Keywords:photocatalysts;g-C3N4;thiophene-amide;embedding;induction effect;delocalization effect;hydrogen evolution
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POLYMER COMPOSITES
·
2022
·Vol. 43
·期 11
·8228-8238
·
IF 3.531
Zhongying Wang,Huan Wang,Xiaomei Shen,Qingfu Wang,Zhiqian Wang,Fanghui Wang,Hong Zhu
In this work, a series of C 3 N 4 /SiO 2 nanohybrids were prepared and incorporated to solution polymerized styrene-butadiene rubber/butadiene rubber (SSBR/BR) to prepare “green tire” tread rubber. As expected, C 3 N 4 /SiO 2 nanohybrids are uniformly dispersed in SSBR/BR, and SiO 2 possesses a small average particle size of ~15 nm. In addition, the interfacial interaction between C 3 N 4 /SiO 2 nanohybrids and rubber matrix are significantly enhanced. Hence, the mechanical properties of C 3 N 4 /SiO 2 -SSBR/BR nanocomposites are greatly improved. The tensile strength of 5% C 3 N 4 /SiO 2 -SSBR/BR nanocomposites (5 wt% C 3 N 4 in C 3 N 4 /SiO 2 ) improved 1580% compared to pristine SSBR/BR. Furthermore, dynamic mechanical analyses indicate the increasing wet skid resistance (10.8% higher) and decreasing rolling resistance (50.5% lower) of 5% C 3 N 4 /SiO 2 -SSBR/BR nanocomposites compared with SiO 2 -SSBR/BR. In addition, the wear volume and heat built-up are reduced at the same time. This work paves the way to prepare high comprehensive performance “green tire” and could be extend to the reinforcement of elastomer composites.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 30
·期 3
·8098-8109
·
IF 5.19
Shan Junyue,Wu Xianliang,Li Caifang,Hu Jiwei,Zhang Zhenming,Liu Huijuan,Xia Pinhua,Huang Xianfei
The photocatalytic degradation of antibiotics requires a good separation efficiency of photogenerated electron–hole pairs and a wide visible light absorption range. Current studies have discussed the successful preparation of ferroferric oxide/graphite carbon nitride/reduced graphene oxide (Fe 3 O 4 /g-C 3 N 4 /rGO). The phase structure and morphology of the Fe 3 O 4 /g-C 3 N 4 /rGO composites were characterized by XRD, HR-TEM, SEM, and EDS. The obtained composites were used to degrade tetracycline hydrochloride (TCH) to evaluate its photocatalytic activity. The effects of four variables on the degradation of TCH were analyzed by the response surface method and artificial intelligence (gradient regression tree, random forest, artificial neural network, etc.). The results showed that the graphite carbon nitride in the catalyst maintained its original structure and that the photocatalytic activity was significantly improved. The degradation rate of TCH was 86.7% under the optimal conditions (the Fe 3 O 4 /g-C 3 N 4 /rGO dosage was 0.1 g, pH = 7.0, the initial concentration of TCH was 20 mg/L, and the visible light irradiation time was 60 min). At the same time, the degradation rate of TCH changed little after the material was used five times, which indicates that the stability and recyclability of the Fe 3 O 4 /g-C 3 N 4 /rGO photocatalyst were excellent. Finally, a possible photocatalytic mechanism of the Fe 3 O 4 /g-C 3 N 4 /rGO photocatalyst is proposed in this paper.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Chengyuan Yang,Jing Wang,Rong Wang,Wenxin Zhu,Liang Zhang,Ting Du,Jing Sun,Ming-Qiang Zhu,Yizhong Shen,Jianlong Wang
Multi-pollutants environment coexisted organic and inorganic pollutants has become a common phenomenon, seriously affecting water biodiversity and human water security. Currently, the removal of organic and inorganic pollutants by photocatalysis are mostly in own single-pollutant environment, not in multi-pollutants system, where the common photocatalysts cannot achieve efficiently charge separate and transfer with low reactive oxygen species (ROS) efficiency. Herein, we constructed an efficient cascaded Z-scheme heterojunction Co 9 S 8 @defective ZnS/g-C 3 N 4 (C@DZ/N) composed of defective engineering in hollow nanocubes, which achieved excellent photodegradation activity (98.93 % for ciprofloxacin (CIP) and 97.18 % for Cr(VI) at 90 min) in multi-pollutants environment, significantly higher than the hollow cubic with Z-scheme heterojunction in single-pollutant environment (98.07 % for CIP and 98.72 % for Cr(VI) at 140 min). Defective ZnS acts as the core for direct charge transfer and separation to form a unique cascaded Z-scheme heterojunction system that blocks the type II charge transfer pathway to achieve ultra-efficient charge transfer. Furthermore, the structural characterization and ROS experimental results based on multi-pollutants models show that the cascade Z-scheme system greatly facilitates the ROS release kinetics and further leads to more electron-deficient cubic surfaces while increase the directional conversion to singlet oxygen ( 1 O 2 ) in multi-pollutants environment. Further tests of intermediates and reusability indicated its potential for the high-efficient treatment of multiple pollution systems.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2022
·
IF 9.221
Cheng Feng,Congting Zhang,Chang Xu,Shuang Lin,Baohua Zhang,Huanxing Wu,Zheng Zhang,Xinming Guo,Haineng Bai,Fuqiang Guo
The detection of H 2 S for biomarkers or special occasions often requires a lower detection limit. In this work, the ppb-level H 2 S sensor based on MoO 3 /CuO/g-C 3 N 4 (MCC) was presented by a simple method. The characterized results show that MCC-2 possesses a larger specific surface area, and has more adsorbed oxygen and oxygen vacancy compared to MoO 3 and MoO 3 /CuO. The gas-sensitive test results show that the response of the MCC-2 sensor to 1000 ppb H 2 S is up to 8.24 at room temperature , which is 1.31 times of MoO 3 /CuO (6.28). More importantly, the theoretical detection limit of the MCC-2 sensor is as low as 1.1 ppb, which is the lowest in the recent H 2 S sensor. In addition, the MCC-2 sensor has reliable repeatability, excellent selectivity to H 2 S, and still maintains a high response after continuous test for 5 weeks. Simultaneously, the MCC-2 sensor also keeps an outstanding response at high relative humidity. The excellent gas sensing properties are due to the larger specific surface area that can enable more gases to be adsorbed on the material surface. In addition, the oxygen vacancy reduces the energy required to adsorb the target gas and the formed heterojunctions by MoO 3 /CuO/g-C 3 N 4 expedite carrier migration.
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