CHINESE JOURNAL OF CATALYSIS
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2022
·
IF 12.92
Yingcong Wei,Qiqi Zhang,Ying Zhou,Xiongfeng Ma,Lele Wang,Yanjie Wang,Rongjian Sa,Jinlin Long,Xianzhi Fu,Rusheng Yuan
Simultaneous generation of H 2 fuel and value-added chemicals has attracted increasing attention since the photogenerated electrons and holes can be both employed to convert solar light into chemical energy. Herein, for realizing UV-visible-NIR light driven dehydrogenation of benzyl alcohol (BA) into benzaldehydes (BAD) and H 2 , a novel localized surface plasmon resonance (LSPR) enhanced S-scheme heterojunction was designed by combining noble-metal-free plasmon MoO 3– x as oxidation semiconductor and Zn 0.1 Cd 0.9 S as reduction semiconductor. The photoredox system of Zn 0.1 Cd 0.9 S/MoO 3– x displayed an unconventional reaction model, in which the BA served as both electron donor and acceptor. The S-scheme charge transfer mechanism induced by the formed internal electric field enhanced the redox ability of charge carriers thermodynamically and boosted charge separation kinetically. Moreover, due to the LSPR effect of MoO 3− x nanosheets , Zn 0.1 Cd 0.9 S/MoO 3− x photocatalysts exhibited strong absorption in the region of full solar spectrum. Therefore, the Zn 0.1 Cd 0.9 S/MoO 3− x composite generated H 2 and BAD simultaneously via selective oxidation of BA with high production (34.38 and 33.83 mmol·g −1 for H 2 and BAD, respectively) upon full solar illumination. Even under NIR light irradiation, the H 2 production rate could up to 94.5 mmol·g −1 ·h −1 . In addition, the Zn 0.1 Cd 0.9 S/MoO 3– x composite displayed effective photocatalytic H 2 evolution rate up to 149.2 mmol·g −1 ·h −1 from water, which was approximate 6 times that of pure Zn 0.1 Cd 0.9 S. This work provides a reference for rational design of plasmonic S-scheme heterojunction photocatalysts for coproduction of high-value chemicals and solar fuel production.
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高影响因子
FUEL
·
2021
·
IF 6.609
Ya-Qi Shan,Lin-Xin Yin,Oraléou Sangué Djandja,Zhi-Cong Wang,Pei-Gao Duan
Ru supported on activated carbon (C), Al 2 O 3 , CeO 2 , MgO, TiO 2 , and ZrO 2 were prepared and employed to boost supercritical water gasification (SCWG) of microalgae hydrothermal liquefaction (HTL) downstream water at 600 °C for 1 h. Effects of catalysts, water density, and Ru/C loading on total organic carbon (TOC) reduction, carbon gasification efficiency (CGE), and gas yield were examined. All the Ru catalysts showed a positive effect on TOC reduction and converted organics in the HTL downstream water to fuel gas, with H 2 and CH 4 as the two most abundant component. With the addition of Ru/C, almost complete removal of TOC, the highest CGE, and H 2 yield were achieved due to its largest metal dispersion. With the addition of Ru/C, increasing water density and catalyst loading favored TOC reduction and CGE increase as well as the total gas yield. The highest H 2 content of 50% and yield of 2.62 mmol/g (aq.) were obtained at the highest catalyst loading of 12.0 mg (Ru/C) /mL (aq.) . This study suggested that SCWG with the addition of Ru/C was a promising strategy to produce fuel gas rich in H 2 , from the organics in the microalgae HTL downstream water.
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RSC Advances
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2020
·Vol. 10
·期 33
·19669-19685
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IF 3.119
Shuting Zhang,Guoqiang Li,Liyuan Duan,Hongyu Wang,Yongle Zhao,Yongfa Zhang
Graphitic carbon nitride (g-C3N4) was prepared by a simple thermal polymerization method in this work. The effects of precursor type, thermal polymerization temperature, constant temperature time and atmosphere on the crystal structure, morphology, elemental composition, valence distribution, light absorption properties and photocatalytic activity of the prepared photocatalytic materials were investigated. Taking rhodamine B (RhB) as the target degradant, the blue light catalytic activity of the photocatalytic material was studied in detail. The experimental results showed that the final pyrolysis temperature and constant temperature time are positively related to the adsorption characteristics and photocatalytic ability of the prepared materials. In addition, the adsorption capacity and photocatalytic activity of the products obtained in Ar and H2 atmospheres are better than those produced in CO and CH4, which can be attributed to the combined effect of large specific surface area and structural defects of the materials. The sample's large specific surface area, wide band gap, and excellent photogenerated carrier separation and transfer capabilities make the adsorption performance and photocatalytic performance of the products obtained with ammonium thiocyanate and thiourea as precursors better than those prepared from melamine and dicyandiamide. g-C3N4 prepared by using ammonium thiocyanate as precursor at 550 °C for 5 h under a hydrogen atmosphere showed the best catalytic activity for the degradation of RhB under blue light. It was demonstrated that g-C3N4 prepared exhibited good stability and reusability after four repeat experiments. The active components that play major roles in the degradation of RhB described herein were holes and superoxide radicals, which was inferred by free radical trapping experiments. This work provides a theoretical basis for the idea of converting the mixed salts of desulfurization waste liquid containing ammonium thiocyanate into an excellent photocatalyst g-C3N4 with visible light response.
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PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2019
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IF 4.175
Man Zhou,Jingwen Chen,Yakang Zhang,Mengting Jiang,Song Xu,Qian Liang,Zhongyu Li
As a typical perovskite-type metal oxide , SrTiO 3 has emerged as prospective candidate for many fields. However, the synthesis of SrTiO 3 with controlled morphology, high surface area, and enhanced photocatalytic activity are still lacking. Herein, a series of porous SrTiO 3 with well-controlled morphologies including assembled nanoparticles (ANPs), golf-like particles (GLPs), star-like microspheres (SLMs), urchin-like microspheres (ULMs), and flower-like microspheres (FLMs) were successfully prepared via an ethylene glycol-water mixed solvothermal route. The ratio of V EG /V H2O play an important role in the shape-evolution during the solvothermal reaction. A comparative study of photocatalytic H 2 production and photodegradation was performed, and a possible photocatalysis mechanism of SrTiO 3 has been proposed. Significantly, the ULMs and FLMs photocatalysts of SrTiO 3 with optimized low Pt loading amount (0.075 wt %) exhibited outstanding H 2 production rates (8.21 and 7.29 mmol g −1 h −1 ) due to its unique structure of high-surface area and defect-rich surface. The facile and shape-controlled synthesis of varied SrTiO 3 structures is believed to be useful for the design and application of perovskite .
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Catalysis Science & Technology
·
2019
·Vol. 9
·期 23
·6627-6637
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IF 5.726
Zhiwei Liang,Yuguo Xia,Guiming Ba,Haiping Li,Quanhua Deng,Wanguo Hou
The high recombination efficiency of photogenerated charge carriers is the primary factor suppressing the photocatalytic performance of polymeric carbon nitride (CN). To enhance the charge separation, Sb-doped CN (CN/Sb) was firstly synthesized using antimonate as a doping and oxidizing agent. The N–SbIII bond was fabricated in CN/Sb via a redox process, which works as a charge-capture center, evidenced by experimental and theoretical calculation methods, and leads to a prominent enhancement in the charge separation and transfer performance of CN/Sb. CN/Sb exhibits much higher photocatalytic activity than CN in water splitting and environmental remediation. The visible-light photocatalytic hydrogen evolution rate of CN/Sb can reach ∼1.75 mmol g−1 h−1, which is ∼4.5 times that of CN, with an apparent quantum yield of 6.4% at 420 nm. Reactive oxygen species generation rates of CN/Sb are also much higher than those of CN. This work provides not only a new effective way for CN modification but also a deep insight into the metal-doping structure in the CN framework, which can guide future research on metal-doped CN photocatalysts.
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Inorganic Chemistry Frontiers
·
2019
·Vol. 7
·期 2
·437-446
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IF 5.934
Yuwei Wang,Xianggui Kong,Meihong Jiang,Fazhi Zhang,Xiaodong Lei
A bifunctional ZnIn2S4/Nb2O5 (ZIS/NbO) photocatalyst was constructed by growing Nb2O5 nanospheres on the petals of ZnIn2S4 microspheres via a facile hydrothermal approach. The composite possessed a direct Z-scheme heterostructure that was confirmed by in situ irradiated X-ray photoelectron spectroscopy (ISI-XPS) and electron spin resonance (ESR) measurements. Owing to the good charge separation efficiency in the Z-scheme system, the lifetime of charge carriers in ZIS/NbO was obviously prolonged. Thus, the rate of hydrogen evolution for optimized ZIS/NbO was 2.8 and 1.8 times higher than that of Nb2O5 and ZnIn2S4, respectively. Furthermore, the ZIS/NbO also showed good performance for the oxidation of biomass-derived intermediate 5-hydroxymethylfurfural (HMF) to value-added products. More importantly, the coupled photocatalytic H2 reduction and HMF oxidation were achieved on the ZIS/NbO Z-scheme heterostructure at the same time. Due to the presence of a direct Z-scheme heterojunction that prevents the recombination of photogenerated electrons and holes in the composite, the ZIS/NbO displayed excellent photocatalytic performance. Our findings are expected to offer a broad optical window for fabricating bifunctional heterostructured composites for coupled photocatalytic reduction and oxidation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Ming Fang,Zhenfei Yang,Yang Guo,Xinnian Xia,Shuaijun Pan
The internal electric field induced by piezoelectric effect can optimize the transport pathway of photogenerated charge in photocatalysis. We constructed an effcient piezoelectric photocatalytic heterojunction UiO-66-NH 2 @CdS and achieved a shift in the charge transfer mechanism through the piezoelectric effect, resulting in excellent photocatalytic H 2 evolution performance. The optimal heterojunction under the ultrasonic environment exhibited 2028.48 μmol·g −1 ·h −1 photocatalytic H 2 evolution performance, roughly four times better than no-ultrasound condition. Because of the piezoelectric polarization of UiO-66-NH 2 , the photogenerated carrier transport mechanism was changed from type Ⅱ to the more favorable Z-scheme for charge separation. Meanwhile, the built-in electric field caused by the piezoelectric effect can act as a powerful driving force for charge separation, achieving high charge separation efficiency and promoting the utilization of photogenerated electrons. This work would provide a fresh perspective for MOF-based piezoelectric photocatalysts and have implications for the design of efficient Z-scheme heterojunctions.
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Catalysts
·
2023
·Vol. 13
·期 7
·1080
·
IF 3.9
Shiyuan Lin,Ruosong He,Wenhang Wang,Yang Wang,Yongqiang Gu,Qiang Liu,Mingbo Wu
The abundant C1 source CO2can be utilized to produce value-added chemicals through hydrogenation technology. A bifunctional catalyst consisting of reducible metal oxide Cr2O3and acidic zeolite ZSM-5 was designed for the direct conversion of CO2+ H2into valuable aromatics, especially para-xylene (PX), via the methanol-mediated pathway. The twin structure of ZSM-5 (ZSM-5T), with sinusoidal channels that are predominantly exposed to the external surface, enhances the possibility of the transformation of methanol into PX due to the favorable diffusion dynamic of PX in the sinusoidal channels. Via the bifunctional catalyst Cr2O3&ZSM-5T, a PX selectivity of 28.7% and PX space-time yield (STY) of 2.5 gCH2h−1kgcat−1are achieved at a CO2conversion rate of 16.5%. Furthermore, we rationally modify the ZSM-5Tzeolite via Cu species doping and amorphous SiO2shell coating (Cu-ZSM-5T@SiO2). After combining with the Cr2O3catalytic component, the CO2conversion (18.4%) and PX selectivity (33.8%) are increased to some extent, which systematically increases the STY of PX to 3.0 gCH2h−1kgcat−1. The physicochemical property of the acidic zeolite and the corresponding structure-function relationship in enhancing the PX productivity are discovered. Our work provides a novel catalyst design idea to boost PX synthesis performance from CO2hydrogenation.Keywords:CO2hydrogenation;bifunctional catalysts;para-xylene;H-ZSM-5 zeolites
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Yuhao Chen,Kaihang Yue,Jia-Wei Zhao,Zhengyang Cai,Xianying Wang,Ya Yan
Constructing low-cost, high-active and robust heterogeneous hydrogen evolution reaction (HER) electrocatalysts with strong metal–metal oxide-support interaction (SMMOSI) is still an urgent challenge for the development of anion exchange membrane water electrolysis (AEMWE), especially under high current density (e.g., 1 A cm −2 ). Herein, a hierarchical composite of heterogenous Ni 4 Mo/NiMoO 4 (NiMoO x ) nanoparticles (NPs) anchored on a mesoporous carbon CMK-3 (NiMoO x @CMK-3) is designed as a superior electrocatalyst for HER. Significantly, the strong interaction between heterogeneous NiMoO x NPs and CMK-3 supporting matrix effectively stabilize the catalytic active Ni 4 Mo/NiMoO 4 heterostructure by altering the local geometric and electronic structures, leading to maximumly exposure of active sites and promoted electron transfer ability. The optimized electrocatalyst exhibits outstanding HER activity with an extremely low overpotential and Tafel slope of 7 mV@10 mA cm −2 and 27.7 mV dec -1 , respectively, and can steadily operate at 100 mA cm −2 for 800 h. More significantly, owing to these HER merits, the AEMWE configuration with NiMoO x @CMK-3 (−) is also designed, resulting in low cell voltage of 1.965 V@1 A cm −2 and negligible degradation over 400 h@1 A cm −2 . Further ex/in-situ electrochemical spectra evidence that both the partial combined MoO 4 2- from NiMoO 4 and the newly formed MoO 4 2- originating from dissolved Mo in NiMoO x @CMK-3 could boost the fast generation of polymerized Mo 2 O 7 2- that could effectively accelerate the HER process in alkaline conditions by facilitating the formation of active Mo-H* intermediates. Moreover, theoretical calculation results demonstrate the upshifting of d-band center of Mo toward Fermi level for the heterogeneous NiMoO x and the strong charge distribution between the heterointerface could optimize adsorption free energies of H* (ΔG H* ) on the surface of Mo atoms.
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Nano Energy
·
2018
·
IF 13.12
Peng Zhou,Fan Lv,Na Li,Yelong Zhang,Zijie Mu,Yonghua Tang,Jianping Lai,Yuguang Chao,Mingchuan Luo,Fei Lin,Jinhui Zhou,Dong Su,Shaojun Guo
Tuning reactive metal-support interaction (RMSI) is a promising approach to optimizing catalytic active sites via the electronic, geometric and compositional effects. In general, the RMSI is conducted on the reducible oxides via a high-temperature reaction (>550 °C). Herein we report a strong RMSI between Pt single atom (PtSA) and non-oxide-based g -C 3 N 4 built by an in-situ photocatalytic reduction method at a sub-zero temperature. The experimental observation confirms that the rich N vacancies in g -C 3 N 4 produce an obvious electron-deficient effect, which greatly enhances the RMSI. This strong RMSI contributes to the highest PtSA coverage density of 0.35 mg m −2 reported to date in carbon-based materials and outstanding H 2 -evolution activity of 174.5 mmol g −1 h −1 per PtSA relative to those on the electron-rich g -C 3 N 4 . The structure simulation reveals that the RMSI can not only stabilize the PtSA on the electron-deficient g -C 3 N 4 via the strong chemical bond between PtSA and the two-coordinated C (C 2C ) sites caused by the N vacancies, but also promises the PtSA with an optimized electronic and geometric structures for capturing photogenerated electrons and producing H 2 . This finding opens a new channel for designing and manipulating single atom-loaded photocatalyst via the RMSI at a sub-zero low temperature.
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ENERGY & FUELS
·
2018
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IF 3.024
Lincai Peng,Xueying Gao,Xin Yu,Hui Li,Junhua Zhang,Liang He
An integrated multistep catalytic process in a one-pot cascade model to realize conversion is preferred in terms of process economics and energy efficiency. Here, we present the noble-metal-free but highly effective catalytic transfer hydrogenation and acid-catalyzed conversion of biomass-derived furfural for direct production of biofuel alkyl levulinate using alcohols as the hydrogen donor and reaction medium. With optimization of the process variables, a high yield of alkyl levulinate at up to 85.3% could be captured under mild conditions in isopropanol medium with the combination of Zr-MCM-41 and Amberlyst-15 catalysts. The reaction proceeds via the catalytic transfer hydrogenation of furfural to furfuryl alcohol over Zr-MCM-41, which is then converted to alkyl levulinate by an Amberlyst-15 acid catalyst. The spent hybrid catalysts could be effectively recovered from the resulting reaction mixture and reused 5 times with little deactivation after plain regeneration treatment.
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高影响因子
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2019
·Vol. 43
·期 8
·3823-3836
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IF 3.343
Xiang Luo,Yu Hong,Honglei Zhang,Kaiqi Shi,Gang Yang,Tao Wu
Summary Steam reforming of ethanol (SRE) over non-noble metal catalysts is normally conducted at high temperature (>600°C) to thermodynamically favour the catalytic process and carbon deposition mitigation. However, high temperature inhibits water-gas shift reaction (WGSR) and therefore restrains the yield of H 2 and leads to the formation of an excessive amount of CO. The modification of non-noble metal catalyst to enhance WGSR is an attractive alternative. In this study, CeO x was firstly loaded onto a nano-scaled Ni x Mg y O matrix and subsequently used as the catalyst for hydrogen production via SRE. Morphology of the catalyst materials was characterized by using a series of technologies, while H 2 -temperature programmed reduction (H 2 -TPR), CO-temperature programmed deposition (CO-TPD), and X-ray photoelectron spectroscopy (XPS), were employed to study the surface nickel, ceria clusters, and their interactions. The catalytic activity and durability of the catalyst were studied in the temperature region of 500°C to 800°C. The CeO x -coated nano Ni x Mg y O matrix exhibited an outstanding hydrogen yield of 4.82 mol/mol ethanol under a high gas hourly space velocity (GHSV) of 200 000 hour −1 . It is found that the unique Ni 0 -CeO x structure facilitates the adsorption of CO on the surface and therefore promotes the effective hydrogen production via WGSR. Moreover, this modified Ni x Mg y O matrix was found to be a more robust and anticoking nanocatalyst because of reversible switch between Ce 4+ and Ce 3+ .
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