Materials
·
2022
·Vol. 15
·期 21
·7464
·
IF 3.748
Ying Yang,Suoying Zhang,Lin Gu,Shijie Hao
Herein, we report a stable catalyst with Ru single atoms anchored on a one-dimensional carbon fiber@graphitic carbon nitride hierarchy, by assembling wet wipes composed of fiber-derived carbon fiber (CF), melamine-derived graphitic carbon nitride (g-C3N4) and RuCl3 before NaBH4 reduction. The atomically dispersed Ru species (3.0 wt%) are tightly attached via N-coordination provided by exterior g-C3N4 nanosheets, and further stabilized by the interior mesoporous CF. The obtained CF@g-C3N4–Ru SAs catalyst can be cycled six times without notable leaching of Ru or loss of GVL yield in the acidic media. This catalyst is more stable than Ru nanoparticles supported on CF@g-C3N4, as well as Ru single atoms anchored on CF and g-C3N4, and proves to be one of the most efficient metal catalysts for aqueous LA hydrogenation to γ-valerolactone (GVL). The isolated Ru atoms by strong N-coordination, and their enhanced electron/mass transfer afforded by the one-dimensional hierarchy, can be responsible for the excellent durability of CF@g-C3N4–Ru SAs under harsh reaction conditions.Keywords:Ru single atom;one-dimensional hierarchy;levulinic acid;γ-valerolactone;stability
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高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Xiaobin Dong,Han Wang,Xiaolong Li,Pedram Fatehi,Shoujuan Wang,Qin Wu,Keyin Liu,Fangong Kong
Graphitic carbon nitride is a very potential photocatalytic catalyst for H 2 production, but its practical application is seriously limited by the fast recombination of photogenerated carriers and insufficient utilization of surface charge. In order to solve these problems, herein, a series of g-C 3 N 4 -NiO-NiS x photocatalysts were synthesized by first calcining the precursor to load NiO on g-C 3 N 4 and subsequently partial sulfidation of NiO into NiS x in situ via a hydrothermal process. Under the irradiation of visible light, the photocatalytic H 2 production rate of g-C 3 N 4 -NiO-0.4T can be up to 1248.1 μmol·g −1 ·h −1 using triethanolamine as sacrificial agent. In addition, recycling test also confirmed g-C 3 N 4 -NiO-0.4T has excellent photostability. It is believed that the formation of p-n junction between NiO and g-C 3 N 4 and the presence of NiS x promote the spatially fast separation of photogenerated carriers, while the abundant interface of NiS 2 and NiS also leads to the good proton trapping ability. These two factors jointly determine the efficient H 2 production of the composite photocatalysts. Furthermore, the detailed energy band structure and plausible photocatalytic mechanism of g-C 3 N 4 -NiO-NiS x are also proposed. This work can offer a new route and useful reference for the design and research of high efficiency composite photocatalysts for H 2 production.
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CRYSTENGCOMM
·
2022
·Vol. 24
·期 28
·5141-5148
·
IF 3.756
Yan Ma,Dianjun Chi,Yuping Tao,Shengjun Liu,Lei Dong,Yu Chen,Lifang He,Kui Zhang
Catalysts with low cost, high efficiency, and no need for precious metal cocatalysts are the key to realizing the maximum utilization of solar energy-efficient hydrogen (H2) production. In this study, a series of graphitic carbon nitride-derived catalysts (g-C3N4/CoP@C) were successfully obtained by in situ phosphating of g-C3N4/Co-BDC. A CoP@C cocatalyst developed with Co-BDC nanosheets as precursors can accelerate the H2 generation of g-C3N4. The close interface between CoP@C and g-C3N4 increased the electron–hole separation efficiency. Moreover, the CoP@C surface carbon accelerated electron transfer and increased the light absorption range. The prepared g-C3N4/CoP@C composite material exhibited H2 production capability up to 1968 μmol g−1 (3 h), approximately 129.9 times that of g-C3N4. Therefore, the CoP@C cocatalyst is proposed as an alternative to non-precious metal cocatalysts based on the findings of the study.
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CHEMOSPHERE
·
2022
·
IF 8.943
Chong Liang,Mingyu Cui,Wei Zhao,Linyang Dong,Shangshang Ma,Xutang Liu,Dingkai Wang,Zhijie Jiang,Fei Wang
Photocatalytic technology has been considered as a promising method to alleviate environmental pollution owing to the dual characteristics of redox. The novel V-based H 5 PMo 10 V 2 O 40 (HPA-2) photocatalyst with Z-scheme heterostructure was constructed. The energy level of HPA-2 matches well with CdS and g-C 3 N 4 (CN) according to Mott-Schottky and UV–Vis diffused reflectance tests, which allows the efficient separation of photogenerated electrons. The optimized CdS/HPA-2/CN showed superior ability in Rhodamine B (RhB) degradation and reduction of Cr (Ⅵ) under visible light irradiation. The maximum rate constant reached 0.092 min −1 for RhB degradation at 60 min and 0.260 min −1 for Cr (Ⅵ) reduction at 20 min, respectively. The photocatalytic mechanism was analyzed by adding scavengers. The effect of active species for RhB degradation was determined as h + > ·O 2 − > ·OH, while ·O 2 − and e − were essential for the reduction of Cr (Ⅵ). Besides, cyclic tests exhibit excellent repeatability and stable structure of CdS/HPA-2/CN after four cycles. Meanwhile, the detailed degradation process of RhB involving de-ethylation, hydroxylation, substitution and decarboxylation was determined according to LC-MS and evaluated by Fukui function calculation. Furthermore, total organic carbon content decreased to 6.2% of the initial value. In this work, as an electron mediator, HPA-2 provides the inspiration for construction of Z-scheme heterojunction , and CdS/HPA-2/CN exhibits enormous potential in the environmental remediation by photocatalysis .
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COLLOIDS AND SURFACES B-BIOINTERFACES
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2022
·
IF 5.999
Lanxin Xu,Yongling Zhang,Jun Zhou,Tao Jiang
The effective monitoring of nucleotides and their metabolites is critical for the prevention of various genetic metabolic diseases. In this aspect, surface-enhanced Raman scattering (SERS) as an ultrasensitive and nondestructive sensing techniques has spurted an attractive prospect. Henceforth, an effective SERS-based analysis of adenosine monophosphate (AMP) as well as adenine was realized here by utilizing an innovative kind of self-cleaning substrate constructed with graphitic carbon nitride and Au nanoflowers (g-C 3 N 4 @Au NFs). Taking advantages of the numerous nanotip-triggered “hotspot” regions of Au NFs as well as the excellent photocatalytic degradation capability of g-C 3 N 4 matrix, the hybrid substrate not only brought about a low limit of detection (LOD) of 5.01 × 10 −10 M, but also yielded an attractive self-cleaning property. Particularly, these fascinating features of the proposed g-C 3 N 4 @Au NFs facilitated a recyclable monitoring of AMP and adenine in serum with reliable sensitivity and stability. The achieved wide linear range from 10 −4 to 1 mg/mL together with the LOD values down to 10 −5 mg/mL all envisioned that it is possible to monitor and investigate human metabolic processes by SERS protocol.
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Journal of Cleaner Production
·
2022
·
IF 11.072
Wenli Yao,Mingzhe Li,Changduo Sun,Yanlong Liu,Mengling Ma,Fengjuan Chen,Lei Zhou,Yian Zheng
Removal of perfluorinated compounds (PFCs) from the environment is a major challenge due to their refractory, persistent and bioaccumulative properties. In this study, trace Co coupled via Co–P coordination and tourmaline (TM) doped g-C 3 N 4 was fabricated (marked as Co/TM/g-C 3 N 4 ) and used as the catalyst for activating peroxymonosulfate (PMS) to remove emerging PFOA under visible light irradiation. Several affecting parameters were systematically investigated, inlcuding Co/TM/g-C 3 N 4 dosage, PMS concentration, initial pH, as well as coexisting Cl − , HC O 3 − , H 2 P O 4 − , N O 3 − and humic acid . Under the conditions of 0.5 g/L Co/TM/g-C 3 N 4 , 2.5 g/L PMS and pH 3.0, the developed synergistic system had the ability for 81.11% removal of PFOA within 4 h, 67.64% removal after the fourth run, and also could be effectively applied in actual water bodies. During the degradation process , π-π*, N–C N and graphite N played the vital role, with the final defluorination rate of 31.12% at 4 h. Free radical quenching and quantitative analysis, as well as electron paramagnetic resonance was used to verify the free radical and non-free radical pathways for PFOA removal, with the findings that S O 4 • − (2.61 μM at 1 h), •OH (0.067 μM at 4 h), O 2 • − , h + , and O 1 2 were involved with possible time-dependent. By liquid chromatography-mass spectrometry analysis, the short-chain intermediates of C3–C7 were proposed and identified. From this study, trace Co coupled and TM doped g-C 3 N 4 demonstrated higher catalytic potential to activate PMS for visible-light synergistic PFOA removal, with the expectation of achieving a cleaner water environment for human beings.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Yaxi Tian,Yan Gao,Qiongqiong Wang,Zhaojin Wang,Rongfeng Guan,Wenyan Shi
Graphitic carbon nitride (g-C 3 N 4 ) photocatalysts are used to achieve photocatalytic activity under visible light, but they suffer from an unprecedented bottleneck period. These photocatalysts have many intrinsic shortcomings, such as their small specific surface area and inefficient separation rate of photogenerated electron-hole pairs. Therefore, changing the morphology and structure of g-C 3 N 4 are essential challenges in addressing these shortcomings. Herein, we propose a novel one-pot method for constructing porous ultrathin g-C 3 N 4 nanosheets . Melamine and potassium gluconate were effectively combined via a supramolecular assembly strategy. As a gas template, potassium gluconate decomposes to produce CO 2 at high temperature. This novel potassium gluconate-cooperative pore generation on g-C 3 N 4 nanosheets method is proposed for the first time. As a result, the PCN-1.4 (the optimum sample of porous ultrathin g-C 3 N 4 nanosheets) photocatalyst has a large surface and a porous layer structure (67.95 m 2 g −1 , 0.3594 cm 3 g −1 ) with abundant nitrogen defects. Furthermore, the porous ultrathin g-C 3 N 4 nanosheets prepared by this method not only have good performance in hydrogen production , but also in TC degradation. On the one hand, the PCN-1.4 sample exhibits an excellent hydrogen production efficiency (2323 μmol.g −1 h −1 ) that is 12 times that of bulk g-C 3 N 4 (192 μmol g −1 h −1 ). On the other hand, compared to the tetracycline hydrochloride degradation efficiency of bulk g-C 3 N 4 of 22 %, PCN-1.4 exhibits a higher degradation rate as high as 83 %. In summary, a new pathway for the generative pore-making is provided to prepare other porous materials.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2022
·
IF 5.141
Wenjing Wang,Xin Xin,Ke An,Yao Chen,Zhanfeng Zhao,Jiangdan Tan,Dong Yang,Zhongyi Jiang
Graphite carbon nitride (g-C 3 N 4 ) has a huge application potential in the photocatalysis field due to its unique conjugated structure. Inspired by the mussel adhesion protein, the cPTA/CNT/CNU (cPTA, carbonized poly(tannic acid); CNT, g-C 3 N 4 prepared by thiourea); CNU, g-C 3 N 4 prepared by urea) nanorod was synthesized by using PTA as the adhesive and template, and thiourea and urea as g-C 3 N 4 precursors. The CNT/CNU isotype heterojunction is assembled on the surface of porous cPTA nanorod, which effectively solves the problem of high photogenerated electron-hole recombination of pure g-C 3 N 4 . The optimal cPTA/CNT/CNU photocatalyst can degrade 95% of rhodamine B (RhB) within 1 h under visible light, which is much higher than CNT, CNU and CNT/CNU. With the conduction band potential difference of cPTA, CNT and CNU, a multistep electron transfer path forms in the cPTA/CNT/CNU, which can accelerate the electron transfer through the interface, thereby increasing the photocatalytic activity.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yang Huang,Xi Luo,Yini Du,Yu Fu,Xujing Guo,Changwu Zou,Yue Wu
The Fenton-like process provides a promising method to produce reactive radicals for the degradation of refractory organic pollutants in environmental remediation. In this study, the iron-doped g-C 3 N 4 (CNF) coupled with H 2 O 2 was applied to enhance the degradation of carbamazepine (CBZ). And the role of CNF was elucidated by experiment and density functional theory (DFT) calculations. The largest CBZ removal efficiency of 99.02% was achieved in acid condition (pH = 3) with the addition of 0.5 g/L 14% CNF and 50 mM H 2 O 2 . Thirteen intermediates were identified based on high performance liquid chromatography coupled with mass spectrometer (LCMS) and DFT calculations. The degradation products of CBZ were mainly protein-like materials with a low humification degree. During the degradation process, H 2 O 2 was preferentially adsorbed on the active Fe-O site of CNF by hydrogen bonding, hence the promoted electron transfer from H 2 O 2 to Fe(III) contributed to the generation of Fe(II). Certain deformation of H 2 O 2 was observed that the O-O bond length increased to about 1.51 Å. As a result, large amounts of radical species (·OH) were generated by H 2 O 2 decomposition, which was responsible for attacking the CBZ molecules and proceeding the degradation reaction.
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高影响因子
TALANTA
·
2022
·
IF 6.556
Yi Wu,Keren Lu,Fubin Pei,Yanghao Yan,Shasha Feng,Qingli Hao,Mingzhu Xia,Wu Lei
The wide clinical application of d -penicillamine (D-PA) makes it inevitably accumulates in the environment, seriously threatening human health and the ecological environment. To better supervisory control D-PA, a highly sensitive and reliable photoelectrochemical (PEC) sensor based on gold nanoparticles (Au NPs) loaded on graphitic carbon nitride sheet and hexagonal NH 2 -UiO-66 composite (g-C 3 N 4 /Au/NH 2 -UiO-66) was synthesized. Tactfully using the strong bonding between D-PA and Au NPs and the effective carrier separation of Z-scheme heterojunction, the designed g-C 3 N 4 /Au/NH 2 -UiO-66 PEC sensor without an extra recognition unit exhibited a selective and sensitive photocurrent to D-PA. With the aid of UV diffuse reflectance spectra (UV-DRs), electron paramagnetic resonance (EPR) characterization, and free radical capture experiments, the electron transfer path of the PEC sensing system was deduced. The proposed g-C 3 N 4 /Au/NH 2 -UiO-66 PEC-based sensor achieved a low detection limit of 0.0046 μM (S/N = 3) with a wide linear response ranging from 10 nM to 400 μM. In addition, its good stability and selectivity also laid a good foundation for practical applications.
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JOURNAL OF POROUS MATERIALS
·
2022
·Vol. 29
·期 5
·1431-1440
·
IF 2.523
Zhang Shixian,Rong Xinshan,Sun Ting,Gao Ping,Liu Jun,Qiu Xuchun,Zhou Xiangtong,Wu Zhiren
An energy-efficient and environmentally friendly nitrogen fixation process is urgently needed to solve problems of high energy consumption and high emissions in the traditional ammonia industry. In this work, a Z-scheme porous g-C 3 N 4 /ZnFe 2 O 4 photocatalyst was synthesized, characterized and employed for N 2 photofixation. Temperature programmed desorption characterization confirmed that the adsorption capacity of nitrogen was improved for the porous structure. From N 2 photofixation evaluation experiments, the highest ammonia production efficiency can reach 147.33 μmol/L within 120 min. Photocatalytic performance is greatly improved because of the increasing of specific surface areas, enhancement of N 2 adsorption ability and synergistic effect of Z-scheme photocatalytic system. In the ammonia production process of the research, visible light is used as energy; N 2 and H 2 O are used as raw materials, which possesses a good application potential due to the advantages of being energy-efficient, environmentally friendly and pollution-free.
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Journal of Materials Research and Technology-JMR&T
·
2022
·
IF 6.267
Linfa Bao,Jingjing Han,Huifang Wang,Renrong Liu,Muqing Qiu,Baowei Hu
In this study, a novel synergistic photocatalyst (Fe 3 O 4 /GO/g-C 3 N 4 composites) were constructed by chemical precipitation of Fe 3 O 4 nanoparticles on surface of GO/g-C 3 N 4 suspension. The characterization results indicated that Fe 3 O 4 /GO/g-C 3 N 4 composites exhibited high efficient separation of photogenerated electron–hole pair, narrow bandgap (∼2.38 eV) and wide absorption range. The incorporation of Fe 3 O 4 significantly increased the photocatalytic performance of GO/g-C 3 N 4 composites due to synergistic effect. More than 90% of U(VI) was photo-reduced by Fe 3 O 4 /GO/g-C 3 N 4 composites within 2 h under visible light irradiation. The trapping experiments and XPS analysis indicated that the photogenerated electrons and superoxide ( ⋅ O 2 ) radicals are responsible for U(VI) removal. These findings indicated that magnetic g-C 3 N 4 composites can be used as excellent candidates for the high efficient removal of U(VI) in actual environmental cleanup.
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