Small
·
2020
·Vol. 16
·期 18
·2000426
·
IF 11.459
Hongzhi Wang,Hongpan Rong,Dong Wang,Xinyuan Li,Erhuan Zhang,Xiaodong Wan,Bing Bai,Meng Xu,Jiajia Liu,Jia Liu,Wenxing Chen,Jiatao Zhang
Here, the photocatalytic CO 2 reduction reaction (CO 2 RR) with the selectivity of carbon products up to 100% is realized by completely suppressing the H 2 evolution reaction under visible light (λ > 420 nm) irradiation. To target this, plasmonic Au/CdSe dumbbell nanorods enhance light harvesting and produce a plasmon-enhanced charge-rich environment; peripheral Cu 2 O provides rich active sites for CO 2 reduction and suppresses the hydrogen generation to improve the selectivity of carbon products. The middle CdSe serves as a bridge to transfer the photocharges. Based on synthesizing these Au/CdSe–Cu 2 O hierarchical nanostructures (HNSs), efficient photoinduced electron/hole (e − /h + ) separation and 100% of CO selectivity can be realized. Also, the 2e − /2H + products of CO can be further enhanced and hydrogenated to effectively complete 8e − /8H + reduction of CO 2 to methane (CH 4 ), where a sufficient CO concentration and the proton provided by H 2 O reduction are indispensable. Under the optimum condition, the Au/CdSe–Cu 2 O HNSs display high photocatalytic activity and stability, where the stable gas generation rates are 254 and 123 µmol g −1 h −1 for CO and CH 4 over a 60 h period.
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高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Fang He,Lan Luo,Zhenxing Wang,Shaoqin Peng,Yuexiang Li
Design of highly condensed g-C 3 N 4 is a prospective way to optimize the photoreactivity of g-C 3 N 4 as it possesses condensed structure with decreased interlayer spacing, which benefits both charge transfer and light harvesting. Herein, we report that novel condensed carbonized-tannic acid (C-TA)/g-C 3 N 4 composites have been acquired via a supramolecular self-assembly of TA and melamine into TA/melamine precursors followed by thermal condensation. The acquired condensed C-TA/g-C 3 N 4 composites present superior visible-light photocatalytic activity for H 2 evolution. The 1 wt% C-TA/g-C 3 N 4 composite shows 4.2 times enhancement of photocatalytic activity for H 2 evolution compared to pristine g-C 3 N 4 . The TA with distinct adhesion properties and functional groups of OH, which is firmly linked with melamine, can confine the melamine inside to promote the condensation to gain more condensed g-C 3 N 4 . The condensed C-TA/g-C 3 N 4 composites with decreased interlayer distance effectively promote charge transfer and photocatalytic H 2 evolution.
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Journal of Materials Chemistry A
·
2022
·Vol. 11
·期 2
·800-808
·
IF 14.511
Yixuan Lv,Dandan Ma,Kunli Song,Siman Mao,Zhetong Liu,Dan He,Xuewen Zhao,Tianhao Yao,Jian-Wen Shi
The gradual depletion of global fossil energy and environmental pollution make the development of hydrogen energy an imminent concern. Two-dimensional g-C3N4 (CN) based heterostructures have attracted considerable research interest in the photocatalytic H2 evolution field, but the unsatisfactory interfacial contact between metal-free CN and other metal oxide/sulfide semiconductors usually results in a low transfer efficiency of charge carriers. Herein, we develop a new homojunction by in situ decoration of CN nanosheets with a C–N compound broken by s-triazine units (abbreviated to BST). The resultant CN/BST homojunction presents significantly enhanced photocatalytic H2 generation (12.47 mmol g−1 h−1), which is about 4 and 33 times higher than that of pristine CN (3.086 mmol g−1 h−1) and BST (0.376 mmol g−1 h−1), respectively. It is revealed that the BST fragments tightly anchored on the CN nanosheets act as electron-trapping agents to rapidly transfer photogenerated electrons from the CN conduction band to generate hydrogen, effectively inhibiting the recombination of photogenerated electrons and holes. The work shows that the construction of a suitable homojunction is an effective way to obtain high photocatalytic activity.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Caiyun Xu,Kaijie Li,Hongbo Yu,Mingxi Liu,Shenghu Zhou
In this work, Pt nanoparticles encapsulated hollow porous silica nanoreactors (Pt@HPSNs) was synthesized in one-pot by a reverse microemulsion system, and they exhibit good catalytic efficiency and stability for semihydrogenations of alkynes . The key design concept is to form Pt hydroxide nanoparticles mixed poly(ethyleneimine) nano-aggregates in water droplets, which further functions as seeds for silica deposition and the void templates to form the central voids. The Pt@HPSNs illustrate a wide adaptability for semihydrogenations of a series of terminal alkynes to the corresponding alkenes at mild reaction conditions, and demonstrate high yields of styrene for semihydrogenation of phenylacetylene, showing good catalytic efficiency for hydrogenation of phenylacetylene to styrene at atmospheric H 2 pressure. The enhanced catalytic performance of Pt@HPSNs are ascribed to their hollow porous nanostructures , where the confinement of Pt nanoparticles in voids increase the structural stability and the confinement effect may increase the collision of reactants and Pt, resulting in improved catalytic efficiency.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Zijun Yu,Fujiang Geng,Mengjie Han,Dudu Li,Zibo Yang,Zhihua Qiao
6FDA-APBIA was in-situ incorporated into the ZIF-9 framework via coordination bonds. • 6FDA-APBIA incorporation effectively increased the ultra-microporous volume of ZIF-9. • polyZIF-9 based MMMs exhibit excellent H 2 /CH 4 and CO 2 /CH 4 separation performance. • pZ9–30 MMM shows 2.2-fold (H 2 /CH 4 ) and 1.4-fold (CO 2 /CH 4 ) selectivity over pure PI. • pZ9–30 MMM has good interfacial compatibility and long-term operational stability. Mixed-matrix membranes (MMMs) have broad application prospects in the field of gas separation, particularly for the efficient separation of H 2 /CH 4 and CO 2 /CH 4 , which is of great significance for hydrogen energy recovery and natural gas purification. This study proposes a strategy to in situ incorporate 6FDA-APBIA polymer into the ZIF-9 framework via coordination bonds, constructing polyimide-based ZIF-9 materials (pZ9) with tunable pore structure. The characterization results confirm that the appropriate incorporation of polymer increased the ultra-microporous volume of ZIF-9 for achieving molecular sieving. Furthermore, pZ9 materials were used as fillers to prepare self-supported MMMs with varying loadings. Notably, the gas permeation tests revealed that the MMM with 30 wt% pZ9 loading exhibited excellent H 2 /CH 4 and CO 2 /CH 4 separation performance (α H2/CH4 ≈ 328.05, α CO2/CH4 ≈ 95.21), both exceeding the corresponding upper bounds. This work provides insights into the design of high-performance MMMs, showing promise for applications in hydrogen recovery and natural gas purification. Download: Download high-res image (100KB) Download: Download full-size image
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ACS Applied Energy Materials
·
2023
·
IF 6.4
Rui Chen,Ying-Ying Wang,Xia Jiang,Ming-Hao Ji,Hao-Yan Shi,Hai-Long Wang,Yan-Xin Chen,Can-Zhong Lu
This article describes a photocatalytic (PC) hydrogen evolution technology that utilizes Pd/LaCoO3/PCN nanocomposites. In the preparation process, a narrow band gap pure LaCoO3 phase was obtained using a template method, which was subsequently combined with Pd-NPs loaded with pCN to form a Z-scheme heterojunction. The formation of this heterojunction resulted in a material with improved charge transfer characteristics and electron well performance. Under visible light irradiation, the composite material demonstrated a higher PC hydrogen evolution activity, resulting in a H2 yield of 40.2 μmol g–1 h–1. This yield represents a 259 times improvement over pure pCN materials, respectively. Furthermore, in the presence of a sacrificial agent, triethanolamine (TEOA), the production of H2 increased compared to methanol, likely due to the more vital binding ability of the amine-containing pCN to TEOA. Finally, the study found that Pd/LaCoO3/PCN nanocomposites displayed excellent stability and reusability during three continuous cycles. These results suggest that this material may become an efficient and sustainable technology for solar fuel production.
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INTERNATIONAL JOURNAL OF REFRACTORY METALS & HARD MATERIALS
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2023
·
IF 3.6
Meng-Chao Li,Lu Wang,Zheng-Liang Xue
The influences of different parameters, such as reaction temperature, yttrium (Y) content, and H 2 concentration, on the particle size and morphological structure of Mo powder prepared via the H 2 reduction of MoO 2 , were investigated in the work. TG, XRD , FE-SEM, laser particle size analysis , model fitting, and orthogonal design experiment methods were adopted to analyze the reaction kinetic and reduction mechanism. The results showed that the optimum conditions for preparing ultrafine Mo powder were recognized as 1073 K, 1 mass% Y content, and a H 2 concentration of 0.000576 mol·cm −2 ·min −1 , which enabled the as-prepared Mo powder with a particle size as small as 107 nm. A new interfacial chemical reaction model with the consideration of reaction temperature, H 2 concentration, and sample thickness, was proposed to analyze the reaction kinetic. It was found that the curves predicted by the model agreed well with the experimental data, with the apparent activation energy extracted to be 94.686 kJ/mol. The effect of different individual parameter on the reaction rate and the possible reduction mechanism were also elucidated.
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高影响因子
ENERGY CONVERSION AND MANAGEMENT
·
2023
·
IF 10.4
Zhicheng Xu,Ningbo Gao,Yan Ma,Weitao Wang,Cui Quan,Xin Tu,Norbert Miskolczi
Biomass utilization is considered a carbon–neutral way to simultaneously tackle the energy crisis and environmental contamination. Challenges still exist to hinder its application, such as low products yield, tar blockage, harsh condition and inferior stability. This paper aims to study whether the newly developed integrated pyrolysis and plasma-catalysis system can be applied into practice of H 2 production from real biomass volatiles, and to understand roles of temperature and catalyst. The experiments were performed in a two-stage reactor embedded with a coaxial dielectric barrier discharge plasma zone. Impacts of operating conditions (i.e. discharge power, steam input, heat supply and catalyst packing) on H 2 production were investigated. The results show that proper input of discharge power and steam can promote H 2 production. Heating supply is recognized as two different effects on plasma-only and plasma-catalysis systems, since reaction temperature elevation acts as inhibitor to plasma characters and cut down the contribution of plasma reforming. After packing bimetallic Ni-Fe/γ-Al 2 O 3 catalyst into plasma, optimal 47.65 mmol/g of H 2 can be attained at reforming temperature of 500 ℃, with synergy effects observed. Plasma-catalysis system also outperformed in tar cracking, tar elimination and stability test, attributed to plasma assistance. This work provides an alternative to construct a new plasma-catalysis process for H 2 production from biomass volatiles or to couple plasma technology with existing biomass conversion industries for preferable energy and fuel production, highlighting its promising commercialization prospects.
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高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2023
·Vol. 34
·期 17
·1-12
·
IF 2.8
Ramya A. Janaki,Shobanadevi N.,Mangaiyarkarasi S. P.,Sankar R.
Promoting the charge separation to improve photocatalytic performance of semiconductor photocatalysts is very important in the field of artificial photosynthesis. Here, a novel MoS 2 /CdS 2D–2D ultrathin nanosheet heterostructure was fabricated via a one-pot solvothermal route. The obtained 2D–2D MoS 2 /CdS nanojunction has not only provided large contact areas, but also shortened the charge-transport distance, resulting in significantly enhanced photocatalytic H 2 evolution property. By optimizing the 2D MoS 2 amounts in the heterojunction, the 5 wt% 2D/2D MoS 2 /CdS heterojunction displayed the maximal photocatalytic H 2 evolution rate of 5566 μmolh −1 g −1 under visible-light irradiation in the presence of lactic acid as the sacrificial reagent, which was 10.1 times higher than that of pristine 2D CdS (516 μmolh −1 g −1 ). Based on the photoelectrochemical and photoluminescence spectra tests, it could be deduced that the charge separation and transfer of 2D/2D MoS 2 /CdS heterojunction were tremendously improved, and the recombination of photoinduced electron–hole pairs was effectively impeded. Moreover, the 2D MoS 2 was used as a co-catalyst to provide the abundant active sites and lower the overpotential for H 2 generation reaction. The current work would offer an insight to fabricate the 2D/2D heterojunction photocatalysts for splitting H 2 O into H 2 .
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Ming Li,Tongyan Ren,Yubao Li,Shuang Li,Ping He,Yao Xiao,Jiufu Chen
In this study, a series of promising binary hybrid heterojunction CdIn 2 S 4 /ZnS (CIS/ZnS) were constructed via a facile hydrothermal method . Credible characterization methods including powder X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and UV–vis diffuse reflectance spectra (DRS) were carried out to investigate the physicochemical properties the as-obtained photocatalysts . Photocatalytic water splitting for hydrogen evolution was performed to evaluate the photocatalytic activity of the photocatalyst. The results indicate that the light-harvesting ability could be markedly enhanced by decorating CdIn 2 S 4 on ZnS microspheres . Compared with the pristine CdIn 2 S 4 and ZnS, the hybrid photocatalysts present more efficient photocatalytic hydrogen production performance. Among composite photocatalysts, the 5% CIS/ZnS sample manifests the highest photocatalytic hydrogen production rate of 10.80 mmol g −1 h −1 , which is 2.6 and 5.4 times higher than that of ZnS and CdIn 2 S 4 , respectively. Moreover, a type-I band alignment mechanism was prudently put forward to interpret the photocatalytic hydrogen generation activity. The boosted photocatalytic hydrogen evolution activities of CIS/ZnS can be attributed to the enhanced light-harvesting ability, efficient separation and transfer of the photo-induced charge carriers, and inhibition of electrons and holes recombination of binary hybrid CIS/ZnS photocatalysts.
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Nano Research
·
2023
·Vol. 16
·期 5
·6568-6576
·
IF 9.9
Zhang Genrui,Li Xiaojing,Li Na,Wu Tingting,Wang Lei
Constructing 2D/2D face-to-face heterojunctions is believed to be an effective strategy to enhance photocatalytic performance due to the enlarged contact interface and increased surface active sites. Herein, 2D porous NiCo oxyphosphide (NiCoOP) was synthesized for the first time and coupled with graphitic carbon nitride (g-C 3 N 4 ) nanosheets to form 2D/2D heterojunctions via an in-situ phosphating method. The optimal 4 wt.% 2D/2D NiCoOP/g-C 3 N 4 (OPCN) photocatalyst achieves a hydrogen evolution rate of 1.4 mmol·h −1 ·g −1 , which is 33 times higher than that of pure g-C 3 N 4 . The greatly improved photocatalytic performance of the composite photocatalysts could be attributed to the formation of interfacial surface bonding states and sufficient charge transfer channels for accelerating carrier separation and transfer and the porous structure of NiCoOP nanosheets with abundant surface active sites for promoting surface reactions. Amazingly, the 2D/2D OPCN composite photocatalysts also exhibit superior stability during photocatalytic reactions. This study not only designs new noble-metal-free NiCoOP/g-C 3 N 4 composite photocatalysts but also provides a new sight in fabricating face-to-face 2D/2D heterojunctions for their application in energy conversion areas.
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Journal of the Taiwan Institute of Chemical Engineers
·
2023
·
IF 5.7
Meng Chen,Huawei Fang,Chao Wang,Jixiang Xu,Lei Wang
Background Solar-driven water splitting is regarded as one promising green way to produce H 2 . Photo-reduction of hexavalent chromium (Cr(Ⅵ)) to hypotoxic Cr(III) can control the Cr(VI)-induced pollution. A key in these processes is to develop a photocatalyst with high specific surface area, good light absorption and efficient charge carrier separation. Methods A Co-encapsulated N-doped carbon (Co@NC) was prepared by pyrolysis ZIF-8@ZIF-67 precursor to modify CdSe quantum dots (QDs). The obtained catalyst was used to reduce Cr(Ⅵ) and split water under visible light irradiation. Significant findings Modification CdSe with Co@NC made obtained Co@NC/CdSe possessing enhanced visible-light absorption and photoexcited charge separation. The optimal 2%Co@NC/CdSe exhibited the excellent Cr(Ⅵ) reduction performance with a rate constant of 0.28 min –1 in the absence of sacrificial agent, as well as high H 2 evolution rate of 6.48 mmol g –1 h –1 in 10% lactic acid solution. The H 2 O 2 and electrons were the active species to reduce Cr(VI). This work gives a beneficial insight for improving the photocatalytic activity of QDs.
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