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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Enhanced electron–hole separation in SnS2/Au/g-C3N4 embedded structure for efficient CO2 photoreduction

Shikang Yin,Linlin Sun,Yaju Zhou,Xin Li,Jinze Li,Xianghai Song,Pengwei Huo,Huiqin Wang,Yongsheng Yan

The use of semiconductor photocatalytic reduction technology has higher efficiency and lower energy consumption for CO 2 reduction, but its existence of some mismatched energy band positions and relatively slow charge-hole separation greatly limits its practical application. In this paper, a SnS 2 /Au/g-C 3 N 4 embedded structure model with carbon and nitrogen hybridization is proposed to gain an in-depth understanding of the role of hybridization and precious metal modification in photocatalysis. Carriers were investigated from the perspective of kinetics through photocurrent, LSV curve, and FL spectroscopy. After modification of Au nanoparticles, the photo-excited electrons showed a slower decay process, indicating that the separation of carriers was enhanced, which was further confirmed by impedance and PL spectroscopy. SEM, AFM and TEM analysis confirmed that the 2D face-to-face SnS 2 /Au/g-C 3 N 4 embedded structure was successfully prepared and the Au nanoparticles were evenly distributed. Au nanoparticles not only act as a bridge for electron transport in 2D semiconductor materials to accelerate electron transport, but generate more excited electrons by themselves under the radiation of sunlight, which effectively improves the separation efficiency of electron-hole pairs and enhances the photocatalyst activity. DFT calculations show that the Z-type mechanism and the intercalated energy level of the SnS 2 /Au/g-C 3 N 4 embedded structure expand the light absorption and improve the carrier separation efficiency. As expected, the photocatalyst activity with CO and CH 4 the evolution rate of up 93.81 µmol·g −1 ·h −1 and 74.98 µmol·g −1 ·h −1 under visible light irradiation, respectively, while the photocatalytic activity is negligible loss after 30 h photoreduction. This work reveals the role of embedded structure and precious metal modification in the separation and transmission of electron-hole, opening up new perspective for achieving high-efficiency solar CO 2 reduction performance.

CAS / MDL: 7631-95-0
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Green Energy & Environment · 2020 · IF 6.395

Ultra-small UiO-66-NH2 nanoparticles immobilized on g-C3N4 nanosheets for enhanced catalytic activity

Zhuizhui Su,Bingxing Zhang,Xiuyan Cheng,Fanyu Zhang,Qiang Wan,Lifei Liu,Xiuniang Tan,Dongxing Tan,Lirong Zheng,Jianling Zhang

UiO-66-NH 2 , an important metal–organic framework, is usually synthesized by solvothermal method and the particle size is generally larger than 200 nm, which limits its catalytic applications in chemical reactions. It is very meaningful to produce UiO-66-NH 2 nanoparticles with ultra-small size, but remains challenging. Herein, we synthesized UiO-66-NH 2 nanoparticles in size of 8–15 nm that are immobilized on g-C 3 N 4 nanosheets. Compared with the UiO-66-NH 2 synthesized by the traditional solvothermal method (> 200 nm), the ultra-small UiO-66-NH 2 nanoparticles immobilized on g-C 3 N 4 have more unsaturated coordination positions and increased Lewis acidity. Owing to these combined advantages, the ultra-small UiO-66-NH 2 nanoparticles exhibit greatly improved catalytic activity for Meerwein–Ponndorf–Verley reaction than larger UiO-66-NH 2 particles.

CAS / MDL: 13520-92-8
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ELECTROCHIMICA ACTA · 2020 · IF 6.215

SnS2/g-C3N4/graphite nanocomposites as durable lithium-ion battery anode with high pseudocapacitance contribution

Yong Zuo,Xijun Xu,Chaoqi Zhang,Junshan Li,Ruifeng Du,Xiang Wang,Xu Han,Jordi Arbiol,Jordi Llorca,Jun Liu,Andreu Cabot

Tin disulfide is a promising anode material for Li-ion batteries (LIB) owing to its high theoretical capacity and the abundance of its composing elements. However, bare SnS 2 suffers from low electrical conductivity and large volume expansion, which results in poor rate performance and cycling stability. Herein, we present a solution-based strategy to grow SnS 2 nanostructures within a matrix of porous g-C 3 N 4 (CN) and high electrical conductivity graphite plates (GPs). We test the resulting nanocomposite as anode in LIBs. First, SnS 2 nanostructures with different geometries are tested, to find out that thin SnS 2 nanoplates (SnS 2 -NPLs) provide the highest performances. Such SnS 2 -NPLs, incorporated into hierarchical SnS 2 /CN/GP nanocomposites, display excellent rate capabilities (536.5 mA h g −1 at 2.0 A g −1 ) and an outstanding stability (∼99.7% retention after 400 cycles), which are partially associated with a high pseudocapacitance contribution (88.8% at 1.0 mV s −1 ). The excellent electrochemical properties of these nanocomposites are ascribed to the synergy created between the three nanocomposite components: i) thin SnS 2 -NPLs provide a large surface for rapid Li-ion intercalation and a proper geometry to stand volume expansions during lithiation/delithiation cycles; ii) porous CN prevents SnS 2 -NPLs aggregation, habilitates efficient channels for Li-ion diffusion and buffer stresses associated to SnS 2 volume changes; and iii) conductive GPs allow an efficient charge transport.

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MICROCHIMICA ACTA · 2020 ·Vol. 187 ·期 3 ·1-10 · IF 6.232

Electrochemiluminescence immunoassay for the prostate-specific antigen by using a CdS/chitosan/g-C3N4 nanocomposite

Huang Bo,Liu Xing-Pei,Chen Jing-Shuai,Mao Chang-jie,Niu He-Lin,Jin Bao-Kang

An electrochemiluminescence (ECL) biosensor was fabricated for the evaluation of prostate specific antigen (PSA). The sensor was developed by successively modifying glassy carbon electrode (GCE) electrodes with CdS/Chito/g-C 3 N 4 nanocomposites and DNA1 was labeled at the 5′ end with thiol. The aptamer DNA was labeled at the 3′ end with a quencher ferrocene (Fc) was ligated to DNA1 by the principle of complementary base pairing. In the absence of PSA, the ECL intensity signal is effectively quenches through the energy transfer and photoexcitation electron transfer between CdS/Chito/g-C 3 N 4 emitter and quencher Fc. After incubation with target PSA, the aptamer DNA interacts with PSA and then moved away from the electrode surface together, which will recover the ECL intensity. Under the optimal conditions, the ECL intensity increases linearly with the logarithm of PSA concentration in the range of 1 pg·mL −1 to 100 ng·mL −1 , and the detection limit is 0.14 pg·mL −1 (S/ N  = 3). The biosensor has been successfully applied to the determination of PSA in serum sample. Schematic representation of the electrochemiluminescence sensor based on a CdS/chitosan/g-C 3 N 4 nanocomposite, which can be applied to the determination of prostate specific antigen in serum.

CAS / MDL: 7440-43-9 9012-76-4
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2020 · IF 16.683

Z‐scheme photocatalytic production of hydrogen peroxide over Bi4O5Br2/g-C3N4 heterostructure under visible light

Xuesong Zhao,Yingying You,Shaobin Huang,Yixiao Wu,Yiyang Ma,Guan Zhang,Zhenghua Zhang

Photocatalytic production of hydrogen peroxide from water and oxygen is a promising technique due to the green and sustainable solar-to-chemical energy conversion. However, in the absence of organic sacrificial agents as electron donors, the relatively low photocatalytic H 2 O 2 productivity is still far from satisfactory. Herein, we present a Z‐scheme photocatalytic production of hydrogen peroxide over Bi 4 O 5 Br 2 /g-C 3 N 4 heterostructure under visible light without additive organics. The obtained Bi 4 O 5 Br 2 /g-C 3 N 4 heterostructure exhibited a highest H 2 O 2 production of 124 μM in 60 min by a Z-scheme photocatalytic mechanism. The photoinduced electrons of Bi 4 O 5 Br 2 combine with the holes of g-C 3 N 4 at the contact interface, and the e − and h + of the heterostructure are mainly derived from the conduction band of g-C 3 N 4 and valence band of Bi 4 O 5 Br 2 , respectively. As such, more e − and h + of Bi 4 O 5 Br 2 /g-C 3 N 4 heterostructure are available to reduce oxygen and oxidize water, respectively, with more ·O 2 − and ·OH generated and thus more H 2 O 2 produced.

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MATERIALS RESEARCH BULLETIN · 2020 · IF 4.019

Synthesis of high-efficient g-C3N4/polydopamine/CdS nanophotocatalyst based on bioinspired adhesion and chelation

Dong Yang,Wenjing Wang,Xuyang Zhao,Zhiyuan Zhou,Hanjie Ren,Yao Chen,Zhanfeng Zhao,Ke An,Zhongyi Jiang

By utilizing the bioinspired adhesion and metal chelation of polydopamine (PDA), a kind of ternary nanocomposites that consist of the graphitic carbon nitride nanosheet (CNNS), PDA layer and cadmium sulfide (CdS) nanocrystals were synthesized. In the resultant CNNS/PDA/CdS nanocomposites, CdS nanocrystals about 5−10 nm in diameter are scattered on the CNNS surface in the presence of the PDA layer. Due to the energy band matching, CNNS constructs a type II heterostructure with CdS nanoparticles via the mediation of the electroconductive PDA layer, thus enhancing the photocatalytic activity. Compared with pristine CdS and CNNS, the CNNS/PDA/CdS nanocomposite conspicuously shows superior photocatalytic performance under visible light above 420 nm, which can degrade 97 % Rhodamine B (RhB) molecules within 80 min. The introduction of a PDA layer between CNNS and CdS not only promotes the photon energy absorption but also facilitates the separation of photoinduced electron-hole pairs.

CAS / MDL: 62-31-7
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2020 · IF 7.489

Synthesis of EDTA-bridged CdS/g-C3N4 heterostructure photocatalyst with enhanced performance for photoredox reactions

Yi Xiao,Ting Wang,Ganhua Qiu,Kun Zhang,Changguo Xue,Benxia Li

Photocatalytic reactions represent a kind of green and sustainable chemical processes for organic transformations, but the efficiency is limited by the severe recombination and/or inadequate redox potentials of photoinduced charge carriers in photocatalysts . To address these issues, herein, the CdS-EDTA/g-C 3 N 4 heterostructures were designed according to Z-scheme photocatalytic mechanism and synthesized by the hydrothermal growth of CdS on g-C 3 N 4 nanoflakes with assistance of EDTA chelating agent. EDTA played multiple roles in the formation of CdS-EDTA/g-C 3 N 4 heterostructure photocatalysts, such as controlling the morphology of CdS nanostructures , linking CdS and g-C 3 N 4 together, and boosting the charge transfer between two semiconductors. The optimized CdS-EDTA/g-C 3 N 4 (10%) photocatalyst exhibited much higher activities toward the selective reduction of nitrophenol and the selective oxidation of benzyl alcohol , than those of CdS/g-C 3 N 4 heterostructures without EDTA. The enhanced photocatalysis of CdS-EDTA/g-C 3 N 4 can be ascribed to the efficient separation and suitable photoredox potentials of photoexcited charge carriers in the EDTA-bridged Z-scheme system. This work provides the inspiration for exploring inexpensive organic electron mediators for constructing all-solid-state Z-scheme photocatalysts and demonstrates the enhanced performance of Z-scheme photocatalysts for photoredox reactions of organic transformations.

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APPLIED SURFACE SCIENCE · 2020 · IF 6.182

In-situ generation of g-C3N4 on BiVO4 photoanode for highly efficient photoelectrochemical water oxidation

Siyuan Li,Yi Jiang,Wenchao Jiang,Yu Zhang,Kai Pan,Song Wang,Chongyang Hu,Lu-Hua Zhang,Lixin Xia

Constructing a heterojunction photoelectrode is an effective way to promote the photogenerated charge separation in photoelectrochemical (PEC) water oxidation. In this work, we successfully fabricated C 3 N 4 /BiVO 4 hybrid electrodes by integrating g-C 3 N 4 onto the nanoporous BiVO 4 via a simple in-situ synthesis method. The as-prepared C 3 N 4 /BiVO 4 photoanodes were systematically studied by Electrochemical Impedance Spectroscopy, steady-state surface photovoltage (SPV), transient SPV, Open circuit potential and Photoluminescence measurements. With an optimal loading of g-C 3 N 4 , the 2-C 3 N 4 /BiVO 4 electrode showed a high photocurrent density of 4.06 mA/cm 2 at 1.23 V (vs. RHE) for water oxidation, a 2.8 times enhancement over that of the BiVO 4 . It is found that g-C 3 N 4 improved the PEC performance of the photoanodes by simultaneously promoting the charge separation and surface reaction kinetics. When a NiOOH co-catalyst was immobilized onto the 2-C 3 N 4 /BiVO 4 electrode, both the PEC property and stability of the photoanode were enhanced. An extremely high photocurrent density of 5.44 mA/cm 2 at 1.23 V was achieved. The largest half-cell solar energy conversion efficiency for NiOOH/2-C 3 N 4 /BiVO 4 was 1.43% at 0.78 V, corresponding to 8.4 times that of unmodified BiVO 4 (0.17% at 0.97 V). This work brings new insight into the development of C 3 N 4 -based devices for application in solar to fuel conversion.

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COMPOSITES PART B-ENGINEERING · 2021 · IF 9.078

Ultrahigh-performance visible-light photodegradation enabled by direct Z-scheme AgI/(Na,F)–C3N4 composites

Saipeng Zhou,Mingming Hou,Yulong Sun,Wenzhe Zhao,Honglin Wang,Quanhui Guo,Xin Yu,Xinqi Ma,Junwei Zhao

Preparation of high-performance semiconductor photocatalysts is often considered to be the challenge and focus in dealing with water contaminations, and attracts numerous concerns and research interests nowadays. In this work, high-performance Z-scheme AgI/(Na,F) doped g-C 3 N 4 composites were synthesized by facile calcination and in-situ deposition methods and employed for ultrahigh-performance degradation of broad-spectrum antibiotics contaminants. The prepared (Na,F) doped g-C 3 N 4 showed narrower bandgaps, enhanced solar-light absorption, and highly improved visible-light photocatalytic performance. Besides, the strong combined interfaces between AgI nanoparticles and (Na,F) doped g-C 3 N 4 was contributing to visible-light harvesting and highly boosted charge separation of the samples, among which AgI/(Na,F)–CN-40% composite presented the best visible-light photocatalytic performance. The photocatalytic reaction rate constant of the AgI/(Na,F)–CN-40% composite was as high as approximately 0.2007 min −1 , which was 65.80 times of pristine g-C 3 N 4 and 3.60 times of AgI, mainly because of the construction of direct Z-scheme charge transfer pathways between AgI and (Na,F) doped g-C 3 N 4 . Finally, the radical scavenger experiments, possible degradation pathways , and photocatalytic mechanism were also proposed.

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APPLIED SURFACE SCIENCE · 2021 · IF 6.707

Efficient photothermal catalytic CO2 reduction to CH3CH2OH over Cu2O/g-C3N4 assisted by ionic liquids

Pengyan Li,Li Liu,Weijia An,Huan Wang,Wenquan Cui

Photocatalytic CO 2 reduction is a potential way to address simultaneously environmental pollution and energy shortage. However, the difficulties of CO 2 activation and C C coupling lead to quite low conversion efficiency of CO 2 to C2 products. In this study, we constructed Cu 2 O/g-C 3 N 4 heterojunction for photocatalytic CO 2 reduction to ethanol by coupling thermal field and ionic liquids (ILs). The ethanol rate reached 0.71 mmol·g −1 ·h −1 over Cu 2 O/g-C 3 N 4 under photothermalcatalysis, which is 1.89 times that of photocatalysis and 7.05 times that of thermal catalysis. The temperature enhanced thermal motion of the radical, which promotes the formation of ethanol through the ·CH 3 dimerization. The 1-aminopropyl-3-methylimidazolium bromide ILs shows superior CO 2 reduction performance with a high current density (21.3 mA·cm −2 ) than KHCO 3 electrolyte (12.8 mA·cm −2 ). The overpotential is reduced by 0.34 V, which accelerates CO 2 reduction by reducing polarization. It is found that the ILs played a key role in suppressing H 2 O reduction and increasing ethanol yield in this photothermalcatalytic strategy.

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Catalysis Science & Technology · 2021 ·Vol. 11 ·期 23 ·7727-7739 · IF 6.119

g-C3N4/CoNiFe-LDH Z-scheme heterojunction for efficient CO2 photoreduction and MB dye photodegradation

Biao Zhu,Qianxin Xu,Xiaoyan Bao,Dawei Lu,Hao Yin,Yumei Qin,Xing-Can Shen

The development of efficient and stable photocatalysts to solve environmental issues is essential and remains a big challenge. In this work, flower-like CoNiFe-LDH is deposited in situ on g-C3N4 nanosheets, successfully constructing a Z-scheme heterojunction CoNiFe-LDH/g-C3N4 photocatalyst for the photoreduction of CO2 and photodegradation of MB dye. The synthesized nanohybrid shows superior photocatalytic CO2 performance (42.04 μmol g−1 h−1) and fast photodegradation MB performance (0.1057 min−1). The improved photocatalytic performance was attributed to the formation of the Z-scheme heterojunction with matched energy bands, and the intimate heterojunction contact interface, which significantly enhanced the interfacial charge transfer rate and improved the separation efficiency of electron–hole pairs. Moreover, the photocatalytic mechanism was proposed based on PL, photocurrent responses, EIS, and EPR experiments. This work can shed light on further application for environmental problems of Z-scheme heterojunction photocatalysts.

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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Highly-efficient degradation of triclosan attributed to peroxymonosulfate activation by heterogeneous catalyst g-C3N4/MnFe2O4

Jing Wang,Min Yue,Yuze Han,Xing Xu,Qinyan Yue,Shiping Xu

The g-C 3 N 4 /MnFe 2 O 4 as recyclable catalyst was synthesized via auto-combustion sol-gel method. Peroxymonosulfate (PMS) activation by the catalyst for triclosan (TCS) degradation was investigated considering the activation performance, reaction parameters and activation mechanism. The catalyst prepared with 1:1 of g-C 3 N 4 and MnFe 2 O 4 molar ratio performed the best catalytic activity in the TCS degradation and with lest metal leaching. The concentration of Cl − showed a dual effect on the TCS degradation, while HCO 3 − and SO 4 2− performed inhibitory effect. Sulfate radicals, hydroxyl radicals, superoxide and non-radical single oxygen contributed to the degradation of TCS. Compared with MnFe 2 O 4 /PMS system, few heavy metals were leached from g-C 3 N 4 /MnFe 2 O 4 (1:1)-PMS after each reuse ( Fig. S6 b), suggesting that g-C 3 N 4 was conducive to the stability of g-C 3 N 4 /MnFe 2 O 4 (1:1) catalyst. Dichlorination, hydroxylation, cyclization and other bond breaking reaction were inferred as the TCS degradation pathways. These results demonstrated that g-C 3 N 4 /MnFe 2 O 4 (1:1) was a highly effective and stable catalyst for PMS activation to treat toxic organic pollutants in water.

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