ChemCatChem
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2020
·Vol. 12
·期 21
·5504-5510
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IF 4.853
Zi-Cheng Fu,Joshua T. Moore,Zi-Xin Yang,Jia-Jun Hu,Wen-Fu Fu
Graphical CoP for photocatalysis : Sphericalmesoporous SBA-15-supported CoP nanoparticlecatalysts tuning the highly efficient photocatalytic CO-and H 2 -generating pathways with product selectivity of up to 76.3 %and 99.9 % through switching solvent, respectively, were in situ fabricated by CoP embedded on the surface and interior of the porous s-SBA-15. The highly active spherical hybrid catalysts with diameters of 3–8 μm for robust selective CO 2 photoreduction and hydrogen production by switching solvent, CoP/(i)s-SBA-15 and CoP/(o)s-SBA-15, were in situ synthesized for the first time by incorporating CoP nanoparticles on the interior and outside of the spherical mesoporous Santa Barbara Amorphous (s-SBA)-type material s-SBA-15. CoP/(i)s-SBA-15 has a larger pore diameter of ∼9.5 nm, relative to ∼5.7 nm of CoP/(o)s-SBA-15, and a calculated Brunauer-Emmett-Teller surface area of ∼214 m 2 g −1 compared with ∼336 m 2 g −1 for the latter. In comparison with bare CoP, the composites exhibited excellent catalytic CO- and H 2 -generating performance with product selectivity of up to 76.3 % and 99.9 % through switching solvents containing Ru-based photosensitizer under ambient conditions, respectively. The influences of various solvents and electron donors, as well as the amounts of H 2 O, and catalyst on reaction kinetics for CO 2 reduction and H 2 production, and intrinsic properties of both catalysts were investigated and compared.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
·
IF 4.939
Xiaoming Liu,Xueya Chen,Luping Xu,Binquan Wu,Xinman Tu,Xubiao Luo,Fang Yang,Jun Lin
A series of non-noble metal ultrathin MoS 2 nanosheets modified Mn 0.2 Cd 0.8 S heterostructured composites were prepared by an ultrasonic assisted hydrothermal synthesis process. Comparing with the pristine Mn 0.2 Cd 0.8 S composite, the obtained ultrathin MoS 2 /Mn 0.2 Cd 0.8 S composites exhibited a significantly improved photocatalytic activity for hydrogen evolution from water with visible light response. The optimized photocatalytic activity toward MoS 2 /Mn 0.2 Cd 0.8 S composite is around 8 times of the pristine Mn 0.2 Cd 0.8 S composite. Moreover, the ultrathin MoS 2 /Mn 0.2 Cd 0.8 S composites displayed good photocatalytic stability in the course of photochemical reaction . The excellent photocatalytic activity of the ultrathin MoS 2 /Mn 0.2 Cd 0.8 S composites might be attributed to the formed heterojunctions in composites itself and the sufficient active edge sites in MoS 2 phase. A possible photocatalytic mechanism was tentatively proposed. Considering its excellent photocatalytic activity and good photochemical stability, the obtained ultrathin MoS 2 /Mn 0.2 Cd 0.8 S composite has potential application in photocatalytic hydrogen evolution from water by using solar energy.
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CATALYSIS TODAY
·
2020
·
IF 5.825
Hong Du,Miao Jiang,Xiuyun Ma,Peifang Yan,Z. Conrad Zhang
The rapid consumption of fossil resources and the grim environmental situation encourage the application of renewable and clean energy resources. Conversion of biomass, which is a kind of renewable, CO 2 neutral as well as abundant reserves carbon containing resource, is significantly important. The production of fuels from biomass by means of gasification and Fischer-Tropsch synthesis is one of the most promising routes for industrial applications. The wax-free liquid fuels synthesis directly from H 2 -deficient syngas similar to bio-gas is highly advantageous for reducing investment and operating cost. Thus, the Mn-promoted meso-ZSM-5 supported cobalt catalyst was applied for the production of wax-free liquid fuels by catalytic H 2 -deficient syngas conversion in this study. The performance of the reaction was influenced obviously by Mn content. The cobalt dispersion increased with the addition of Mn, whereas the reduction degree decreased after Mn doping. Then, the balance between the dispersion and reduction degree led to the change in CO uptake followed a volcanic curve. The catalyst with moderate amount of Mn (1 wt%) had the suitable cobalt particle size and the maximum CO uptake. Thus, the highest CO conversion was obtained over Co-1Mn/meso-ZSM-5 catalyst thanks to its maximum exposed active sites. The appropriate amount of Mn addition also resulted in the decreasing of CH 4 selectivity. The highest space time yield of liquid fuels was acquired over the Co-1Mn/meso-ZSM-5 catalyst from H 2 -deficient syngas conversion under the moderate conditions.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Hongcai Su,Ekkachai Kanchanatip,Defeng Wang,Haidan Zhang,Antoni,Ishrat Mubeen,Zhicheng Huang,Mi Yan
Ni/Al 2 O 3 catalyst is the one of promising catalysts for enhancing H 2 production from supercritical water gasification (SCWG) of biomass. However, due to carbon deposition , the deactivation of Ni/Al 2 O 3 catalyst is still a serious issue. In this work, the effects of lanthanum (La) as promoter on the properties and catalytic performance of Ni/Al 2 O 3 in SCWG of food waste were investigated. La promoted Ni/Al 2 O 3 catalysts with different La loading content (3–15 wt%) were prepared via impregnation method. The catalysts were characterized using XRD , SEM, BET techniques. The SCWG experiments were carried out in a Hastelloy batch reactor in the operating temperature range of 420–480 °C, and evaluated based on H 2 production. The stability of the catalysts was assessed by the amount of carbon deposition on catalyst surface and their catalytic activity after reuse cycles. The results showed that 9 wt% La promoter is the optimal loading as Ni/9La–Al 2 O 3 catalyst performed best performance with the highest H 2 yield of 8.03 mol/kg, and H 2 mole fraction of 42.46% at 480 °C. La promoted Ni/Al 2 O 3 catalysts have better anti-carbon deposition properties than bare Ni/Al 2 O 3 catalyst, resulting in better gasification efficiency after reuse cycles. Ni/9La–Al 2 O 3 catalyst showed high catalytic activity in SCWG of food waste and had good stability as it was still active for enhancing H 2 production when used in SCWG for the third time, which indicated that La promoted Ni/Al 2 O 3 catalysts are potential additive to improve the SCWG of food waste.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2019
·Vol. 26
·期 10
·2285-2292
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IF 5.16
Ying Xuan,Huiying Quan,Zhurui Shen,Chenxi Zhang,Xiyuan Yang,Lan-Lan Lou,Shuangxi Liu,Kai Yu
Graphical Oxygen covalent functionalization of elemental photocatalysts : A facile and versatile one-step strategy to endow elemental photocatalysts with promoted charge carrier separation ability and photocatalytic H 2 evolution activity is reported, in which band-gap engineering and heterojunction construction are employed to achieve the oxygen covalent functionalization of amorphous red phosphorus (RP) and in situ modification of CdCO 3 . It is known that the low lifetime of photogenerated carriers is the main drawback of elemental photocatalysts. Therefore, a facile and versatile one-step strategy to simultaneously achieve the oxygen covalent functionalization of amorphous red phosphorus (RP) and in situ modification of CdCO 3 is reported. This strategy endows RP with enhanced charge carrier separation ability and photocatalytic activity by coupling band-gap engineering and heterojunction construction. The as-prepared n CdCO 3 /SO-RP ( n= 0.1, 0.25, 0.5, 1.0) composites exhibited excellent photocatalytic H 2 evolution activity (up to 516.3 μmol g −1 h) from visible-light-driven water splitting ( λ >400 nm), which is about 17.6 times higher than that of pristine RP. By experimental and theoretical investigations, the roles of surface oxygen covalent functionalization, that is, prolonging the lifetime of photogenerated carriers and inducing the negative shift of the conduction band potential, were studied in detail. Moreover, the charge transfer mechanism of these composites has also been proposed. In addition, these composites are stable and can be reused at least for three times without significant activity loss. This work may provide a good example of how to promote the activity of elemental photocatalysts by decorating their atomic structure.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Baogang Fu,Nan Su,Yun Wang,Xiangtong Zhou,Yidong Hu,Hongjun Dong,Chunmei Li
In order to achieve the sustainable production of hydrogen fuel, the heterogeneous photocatalysts with inimitable structure are always desired for the high-efficiency and stable H 2 production reaction from water splitting owing to the perfect structure–activity relationship. In this study, a novel metal-free one-dimensional/two-dimensional (1D/2D) heterojunction is constructed by a series of dissolution and diffusion, recrystallization and in-situ growth, and self-assembly process of 1-pyrene carboxaldehyde (PCHO) nanoribbons on the surface of polymeric carbon nitride (PCN) nanosheets. The obtained 1D/2D heterojunction can realize fast carrier transport along 1D nanoribbons to prevent the recombination of photogenerated carriers at the interface. Furthermore, the intrinsic Z-scheme reaction mechanism within the heterostructure also effectively inhibits electron-hole recombination and isolates the reduction and oxidation sites of the photocatalytic reaction. As a result, the dramatically enhanced photocatalytic hydrogen evolution (PHE) activity is achieved over the 1%-PCHO/PCN sample, the optimal PHE rate of which is approximately 5.4 times that of pure PCN . This work provides the deep insight into the design and exploitation of metal-free heterojunction with unique structure applied in the photocatalytic energy conversion field.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 51
·111039-111050
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IF 5.8
Dong Shiwen,Liu Xuan,Kong Xianxian,Dong Feilong,Yu Yan,Wang Lizhang,Wang Da,He Zhiqiao,Song Shuang
Metal-organic frameworks (MOFs) and covalent organic frameworks (COFs) have been proved as efficient catalysts for photocatalytic hydrogen (H 2 ) evolution, thanks to their tunable functionalities, permanent porosity, excellent visible light response, and physicochemical stability. Herein, a series of photocatalysts (termed NUBC) was fabricated by loading different amounts of Zr-UiO-66-NH 2 (NU) onto a benzoic acid–modified covalent triazine–based framework (BC) based on post-synthetic covalent modification. The resulting NUBC catalysts exhibited a type-II Z-scheme heterojunction structure formed via the amide covalent bonds between the amine groups on NU and carboxyl groups on BC. The optimal loading of NU on BC is 30 wt.% (30NUBC) and the corresponding photocatalytic H 2 evolution rate was 378 μmol h −1 g −1 , almost 445 and 2 times than that of NU and BC, respectively. The synergistic effect between the type-II Z-scheme heterojunctions and amide bonds was conducive to boosting visible light harvesting and facilitating charge transportation and separation. Furthermore, the prepared NUBC catalysts show great reusability and stability. Overall, this work sheds light on the design of novel MOF/COF hybrid materials and provides a systematic exploration of their photocatalytic H 2 evolution properties.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Yan Wang,Shuhang Ren,Yucui Hou,Yuanyuan Zhang,Yaling Li,Wanxiang Zhang,Weize Wu
In this work, a series of novel functionalized deep eutectic solvents (DESs) using 1,1,3,3-tetramethylguanidinium tetrazolate ([TMG][Tetz]) as a hydrogen-bond acceptor (HBA) and azole derivatives as hydrogen-bond donors (HBDs) were synthesized for the capture and catalytic reduction of SO2. [TMG][Tetz]:imidazole (Im) (1:2) DES with favorable stability and reversibility could effectively capture 2000 ppm of SO2. The absorption capacity of [TMG][Tetz]:Im (1:2) DES for 2000 ppm of SO2 was high up to 2.0 mol SO2/mol DES (0.40 g SO2/g DES) at 293.15 K. The results of the UV–vis and FTIR spectra revealed that two kinds of combination existed between SO2 and the DES: charge transfer interaction and chemical interaction. Surprisingly, the absorbed SO2, which was found to form charge transfer complexes with the DES, can be reduced by H2 to elemental sulfur under mild conditions without byproduct and additional catalysts. The yield of elemental sulfur could reach up to 37% at 373.15 K.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 24
·16438-16445
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IF 3.3
Zhiwei Yang,Lijuan Dong,Qian Chen,Zeyi Wang,Jiacheng Cao,Mengwei Dong,Jian Wang,Jian Zhang,Xiao Huang
Although titanium-based MXenes have been widely reported for gas sensing, the effect of crystal stoichiometric variations on the sensing properties has been rarely reported. Herein, stoichiometric polymorphs of titanium carbide MXenes (i.e., Ti3C2Tx and Ti2CTx) loaded with Pd nanodots (NDs) prepared by photochemical reduction were investigated for room-temperature H2 sensing. Interestingly, we found that Pd/Ti2CTx exhibited greatly enhanced sensitivity to H2, along with faster response and recovery rates compared to Pd/Ti3C2Tx. The H2 adsorption induced resistance change in Pd/Ti2CTx was higher than that of Pd/Ti3C2Tx due to the more effective charge transfer at the heterointerface of Pd/Ti2CTx, which was confirmed by shifts of binding energies and theoretical calculation results. We hope this work could be helpful to design more high-performance MXene-based gas sensors.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 23
·7869-7875
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IF 4
Deling Wang,Lu Chen,Yuzhou Xia,Ruowen Liang,Xiyao Liu,Shaoming Ying,Guiyang Yan
Developing novel photocatalysts with an intimate interface and sufficient contact is significant for the separation and migration of photogenerated carriers. In this work, a novel Co@NC/ZnIn2S4 heterojunction with a strong Co–S chemical bond was formed at the interface between Co@NC and ZnIn2S4, which accelerated charge separation. Meanwhile, the recombination of the electron–hole pairs was further restricted by the Co@NC/ZnIn2S4 Schottky junction. The Co@NC (5 wt%)/ZnIn2S4 composite exhibited an H2 evolution rate of 33.3 μmol h−1, which is 6.1 times higher than that of the pristine ZnIn2S4, and Co@NC/ZnIn2S4 showed excellent stability in the photocatalytic water splitting reaction. Its apparent quantum yield reached 38% at 420 nm. Furthermore, the Kelvin probe test results showed that the interfacial electric field formed as the driving force for interface charge transfer was oriented from Co@NC to ZnIn2S4. In addition, the Co–S bond as a high-speed channel facilitated the interfacial electron transfer. This work reveals that in situ formed chemical bonds will pave the way for designing high-efficiency heterojunction photocatalysts.
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ENERGY & FUELS
·
2023
·
IF 5.3
Chao Tang,Guolang Zhou,Jianmei Chen,Jingzhou Yin,Yuxin Li,Cheng Liu,Qiaoqi Li,Tianshi Wang,Ziqiang Wang,Shizheng Wen,Benlin Dai,Feihu Mu,Lili Zhang
Developing nonprecious metal catalysts with fast charge transfer ability, abundant active sites, and easy recovery is of great significance toward sodium borohydride (NaBH4) hydrolysis for hydrogen (H2) production in alkaline solutions. Herein, magnetically separated nitrogen-doped carbon-supported cobalt oxide (CoxOy@NC) nanoparticles were prepared successfully by converting pyrazine-based covalent organic frameworks (COFs). Due to the porous structure and nitrogen-rich characteristics of the precursor, the prepared catalyst CoxOy@NC exhibited good conductivity and charge transfer ability. Cobalt oxide nanoparticles and nitrogen-doped carbon matrix are bonded by the Co–N bond, which makes full use of the conductivity of the substrate and the high activity of the cobalt oxide catalyst. Therefore, CoxOy@NC exhibits an excellent synergistic effect between CoxOy and NC. The H2 generation rate reaches a maximum of 2082.13 mL/min/g from NaBH4 in alkaline solutions. In addition, CoxOy@NC also exhibits good magnetic separation capability, which greatly simplifies the catalyst separation process. Density functional theory (DFT) calculation results indicate that Co2+ is the dominant active component in the heterogeneous catalyst CoxOy@NC. This work broadens new horizons for the development of COFs derivative catalysts for hydrogen production from sodium borohydride hydrolysis.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Chao Liu,Wen Xiao,Guiyun Yu,Qiang Wang,Jiawei Hu,Chenghao Xu,Xinyi Du,Jianguang Xu,Qinfang Zhang,Zhigang Zou
Developing efficient heterojunction photocatalysts that have a high charge carrier separation rate and improved light-harvesting capacity is a crucial step in solving energy crisis and reducing environmental pollution. Herein, we synthesized few-layered Ti 3 C 2 MXene sheets (MXs) by a manual shaking process, and combined with CdIn 2 S 4 (CIS) to construct novel Ti 3 C 2 MXene/CdIn 2 S 4 (MXCIS) Schottky heterojunction through a solvothermal method. The strong interface between two-dimensional (2D) Ti 3 C 2 MXene and 2D CIS nanoplates led to enhanced light-harvesting capacity and promoted charge separation rate. Additionally, the presence of S vacancies on the MXCIS surface helped to trap free electrons. The optimal sample, 5-MXCIS (with 5 wt% MXs loading), exhibited outstanding performance for photocatalytic hydrogen (H 2 ) evolution and Cr(VI) reduction under visible light due to the synergistic effect of enhanced light-harvesting capacity and charge separation rate. The charge transfer kinetics was thoroughly studied using multiple techniques. The reactive species of • O 2 − , • OH and h + were generated in 5-MXCIS system, and e − and • O 2 − radicals were found to be the main contributors to Cr(VI) photoreduction. Based on the characterization results, a possible photocatalytic mechanism for H 2 evolution and Cr(VI) reduction was proposed. On the whole, this work provides new insights into the design of 2D/2D MXene-based Schottky heterojunction photocatalysts for boosting photocatalytic efficiency.
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