INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Rui Hu,Zhishi Qiu,Nan Yang,Tong Zhou,Ke Wang,Yuewen Wu,HanLe Luo,Jin Zhang,Weijie Zhan,Yuandong Shen,Jize Li,Hao Cui,Yumin Zhang,Qingju Liu
Covalent Organic Frameworks (COFs), a new type of photocatalyst, have garnered widespread attention in photocatalytic water splitting for hydrogen evolution. However, the photogenerated electron-hole pairs in COFs are prone to recombination, which limits their performance. To address this issue, in this work, a donor-acceptor 1 -acceptor 2 (D-A 1 -A 2 ) type photocatalyst with dual acceptors is constructed, which loaded with Cu onto the electron acceptor sites of donor-acceptor (DA) COFs TpPa-2. Under visible light irradiation, the hydrogen evolution performance of this catalyst reaches 21.6 mmol/g/h. Using EXAS and XPS techniques, we have determined that Cu is bonded to the oxygen on the electron-accepting site of TpPa-2. In-situ XPS and EPR experiments further confirmed that Cu is an electron acceptor, effectively facilitated the transfer of photogenerated electrons, thereby significantly enhancing the photocatalytic performance. This work provides a strategy for the construction of highly efficient visible-light response COFs photocatalysts.
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ACS Applied Energy Materials
·
2024
·
IF 5.4
Meng-Jie Cui,Imran Muhammad,Tie-Zhen Ren,Abulikemu Abulizi,Ai-Sha Nulahong,Zhi-Jun Ren
In recent years, photocatalytic H2 evolution technology has been one of the hot topics to solve the energy crisis. The Cu3Ni/BaTi4O9 composite through hydrothermal and calcination treatment could provide photoelectrons under light irradiation, intriguing the hydrogen (H2) from water molecules. While pursuing a narrow band gap of such materials cannot rely on a simple composite, a chemical bonding contribution is expected to improve the photoexcited electrons by doping the heteroatoms. In this work, boron (B) doping was used to regulate the electronic structure of BaTi4O9 (BTO) and reduce its band gap. Simultaneously, the influence of calcination temperature on the structure and performance of catalysts was explored according to physical characterizations. Due to this, the B(3)-Cu3Ni/BTO photocatalyst possessed macropores with 1–2 μm diameter and abundant mesopores. Under visible light irradiation, the photocatalytic H2 evolution rate reached 318.06 μmol g–1 h–1 at a B doping level of 3%, as determined by gas chromatography analysis. It is 1.73 times that of the undoped B composite catalyst (184.14 μmol g–1 h–1) under the same conditions. Combining density functional theory calculations and experimental studies, it is confirmed that the B-doped form mainly exists in the form of Ti–O–B in BaTi4O9, reducing its band gap value and improving photocatalytic hydrogen evolution activity.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Xuping Li,Yanwei Li,Xingtang Xu,Xiaohua Wang,Guang Sun,Bo Zhang,Yan Wang,Jianliang Cao
Metal oxide semiconductor (MOS)-based hydrogen (H 2 ) sensor that can work at room or near room temperature has attracted an increasing concern owing to its potential application in hydrogen storage and utilization. Herein, a co-sensitization strategy by La doping and Pd decoration is proposed to realize the detection of H 2 at near room temperature (50 °C) on In 2 O 3 porous nanotubes (PNTs). The In 2 O 3 PNTs were prepared via a solvothermal method and then sequentially doped with La 3+ and decorated with Pd nanoparticles via an immersion, freeze-drying and calcination route and a chemical reduction method, respectively. The results of gas-sensing measurements indicated that after a compositional evolution from In 2 O 3 to La-doped In 2 O 3 (La-In 2 O 3 ) and Pd-decorated La-In 2 O 3 (Pd/La-In 2 O 3 ), the fabricated H 2 sensor showed a higher sensitivity at lower operating temperature. At a near room temperature of 50 °C, the response of the best Pd/La-In 2 O 3 sensor to 50 ppm H 2 was as high as 8.34, increasing about 4.85, 1.20 and 1.15 folds compared to the In 2 O 3 (1.72 at 160 °C), La-In 2 O 3 (6.97 at 150 °C) and Pd/In 2 O 3 (7.24 at 80 °C) sensors, respectively. The sensitization effects and mechanism of La dopant and Pd modifier as well as their synergistic effects were discussed in detail.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Xinglin Jia,Jianan Li,Yuhong Liu,Wenzhong Wang,Yujie Li,Lei Liu,Huabin Chen,Guling Zhang,Sitong Liu,Qing Zhou,Lijuan Wang
A novel CdS/CdSe/Cu 2 O nanorod array (NRA) photoelectrode with cascading charge transport channels was designed for the first time to remarkedly boot photoelectrochemical (PEC) hydrogen generation under visible light illumination with zero bias. This ternary photoelectrode was constructed by modifying CdS nanorod arrays with n-type CdSe and p-type Cu 2 O nanoparticles , successively. In this novel photoanode , CdSe and Cu 2 O with small band gap not merely highly heighten the visible light absorption capacity of CdS, but more importantly integrate with CdS to build cascading charge transport channels at the CdS/CdSe and CdSe/Cu 2 O interfaces, dramatically facilitating the separation and transport efficiency for photoexcited electron and hole pairs. The CdS/CdSe/Cu 2 O NRA photoelectrode gains an obvious hydrogen generation rate of 193.2 μmol·h −1 , 8.2 times higher than that of bare CdS NRA photoelectrode. The remarkably enhanced PEC hydrogen production for the CdS/CdSe/Cu 2 O NRA photoanode can be ascribed to effective solar energy utilization and charge carrier separation.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2014
·
IF 2.93
Weirong Zhao,Zhuyu Ai,Xi Zhu,Meng Zhang,Qiaomeng Shi,Jiusong Dai
(AgNbO 3 ) 1− x (SrTiO 3 ) x samples were successfully employed as photocatalysts for photocatalytic hydrogen evolution under visible light. The samples were characterized by a series of techniques, including X-ray diffractometry, scanning electron microscopy, UV–Vis spectrophotometry , and electrochemistry technology. The band gaps of (AgNbO 3 ) 1− x (SrTiO 3 ) x solid solutions can be tuned continuously from 3.21 to 2.65 eV and the flat-band potentials ( V fb ) can be shifted positively from −0.79 to −0.31 V vs. SHE when x decreased from 1 to 0. Band positions of (AgNbO 3 ) 1− x (SrTiO 3 ) x samples were further testified by density functional theory, suggesting that the band gap narrowing of the solid solutions derived from the hybridization of (Ti 3d and Nb 4d) and (O 2p and Ag 4d) orbital. The photocatalytic activities of samples for H 2 evolution with Pt cocatalyst were evaluated in aqueous methanol solution under visible light irradiation . The highest photocatalytic activity was obtained at (AgNbO 3 ) 0.25 (SrTiO 3 ) 0.75 . Photocatalytic activity in hydrogen evolution of these solid solutions proved to be closely dependent on band structures .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xuyang Li,Yingke Zhang,Shuyi Li,Xiaojing Xing,Xinfeng Cheng,Lin Wang,Xianchao Du,Shuai Li,Dongfang Qiu,Meng Guo
Mixed-matrix membranes (MMMs) show great potential for application in hydrogen separation study. However, the MMMs prepared by the traditional strategy have the imperfect compatibility of the matrix and fillers, and the non-ideal microstructure, undergoing a trade-off between permeability and selectivity. Herein, we report a new in-situ limited filling method to improve the H 2 /CH 4 separation performance of the maleic anhydride grafted polypropylene (MAPP) membranes medicated by a series of cyclodextrins (CDs). The introduction of CDs can better loosen the MAPP microstructure and ensure that the nanocomposite membranes have excellent H 2 permeabilities. The two-time limited filling can further compensate for the microvoids or defects in the membrane microstructure, thereby improving the H 2 /CH 4 separation stability of the nanocomposite membranes. The H 2 /CH 4 selectivities of the α-CD/MAPP, β-CD/MAPP, MEDβCD/MAPP, and γ-CD/MAPP are 7.1, 5.7, 6.3, and 5.1 times higher than that of pure MAPP membrane, respectively. This work provides a straightforward and effective strategy to fabricate homogeneous MMMs for gas separation.
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Small
·
2024
·
IF 13
Qiaona Liu,Xin Han,An Qian,Jiayu Qian,Xin Pu,Lei Ye,Jinshan Zhan,Jian Zhang,Qiang Yang,Jichang Liu
Building heterojunctions and exposing more catalytic active sites are effective strategies to enhance the photocatalytic hydrogen evolution activity. Herein, TiO 2 nanosheets are oxidized in situ on Ru-loaded MXene as carriers and subsequently loaded with uniform 2D CdS via hydrothermal method to obtain 2D Ru/Ti 3 C 2 -TiO 2 /CdS composite photocatalysts that integrate heterojunctions and cocatalysts. The formation of heterojunction between CdS and TiO 2 is conducive to promoting the separation and transfer of photogenerated charges, simultaneously, Ru/Ti 3 C 2 with the fully exposed Ru and Ti 3 C 2 can act as effective active sites of photocatalytic hydrogen production reaction. The composite photocatalyst exhibits an improved hydrogen production rate with 5479 µmol g −1 h −1 , which is 5, 3, and four times more than that of pristine CdS, CdS loaded Ti 3 C 2 -TiO 2 and CdS loaded Ru-TiO 2 respectively. The results reveal that the notable enhancement in performance can primarily be ascribed to the introduction of the TiO 2 /CdS heterojunction and the efficient cocatalysts of Ru/Ti 3 C 2 . Moreover, the 2D Ti 3 C 2 with high conductivity as carriers can increase charge transfer, and its 2D structure can serve as a template for growing 2D photocatalysts with higher activity. The interface engineering with multiple interfaces can offer novel insights for the advancement of efficient hydrogen evolution reaction catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Wei Du,Zhihua Zhang,Jundi Wang,Nan Song,Xuezhi Duan,Xinggui Zhou
Propylene epoxidation by H 2 and O 2 to propylene oxide (HOPO), as a novel method for PO production, has attracted widespread attention due to its economic and environmental advantages. Acrolein is a notable byproduct arising in HOPO reaction over Au/TS-1 catalyst, and is traditionally thought to be exclusively formed on Au site through propylene oxidation. However, on the intraporous and external surface Au sites of Au-Ti catalysts, the HOPO reaction have been shown to proceed by different mechanisms, yet the effect of active sites distribution on acrolein formation is far from being understood. Herein, we found that the reaction orders in acrolein formation on Au/TS-1 catalyst (H 2 , 0.19; O 2 , 0.44; C 3 H 6 , 0.44) relative to Au/TS-1 with blocked pores (Au/TS-1-B) catalyst (H 2 , −0.36; O 2 , 0.61; C 3 H 6 , 0.52) were quite different, suggesting a variation in the reaction pathway on the catalysts with different Au locations. Moreover, it is found that PO can be converted to acrolein by O 2 on TS-1 zeolite, which is absent on TS-1-B zeolite without micropores. Consequently, acrolein formation on Au/TS-1 catalyst can proceed through two parallel pathways: propylene hydro-oxidation on Au site, and PO conversion by O 2 inside micropores. Furthermore, by designing and preparing the Au/TS-1 catalysts with different structures, the Au locations are closely related to acrolein formation mechanism and kinetic behaviors. This work provides kinetic insights into the acrolein formation pathways in the HOPO reaction on Au/TS-1 catalyst, and is helpful to the rational design and preparation of efficient catalysts with high selectivity.
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ACS Sensors
·
2024
·
IF 8.2
Shuai Nie,Jing Li,Yunxia He,Xitao Yin
Metal oxide semiconductor gas sensors have demonstrated exceptional potential in gas detection due to their high sensitivity, rapid response time, and impressive selectivity for identifying various sorts of gases. However, selectively distinguishing CH4 from those of CO and H2 remains a significant challenge. This difficulty primarily stems from the weakly reducing nature of CH4, which results in a low adsorption response and makes it prone to interference from stronger reducing gases in the surroundings. Herein, we synthesized In2O3-xCuO nanocomposites using a hydrothermal method to explore their gas sensing properties toward CH4, CO, and H2. Characterization tests confirmed the successful preparation of In2O3-xCuO nanocomposites with different In:Cu molar ratios and the formation of a p-n heterojunction. The gas sensing test results indicated that the In2O3-2.1CuO nanocomposites calcined at 500 °C and measured at 350 °C displayed a p-type response for CH4 and an n-type response for CO and H2, allowing for accurate differentiation of CH4 from CO and H2. Moreover, the In2O3-2.1CuO sensor also showed excellent stability and reproducibility across all three gases. First-principles calculations revealed distinct changes in the electronic structure of the In2O3-CuO heterojunction upon adsorption of CH4, CO, and H2, a finding that aligns with empirical evidence. The gas selectivity mechanism was effectively explained by variations in the energy band gap, driven by electrical behavior during the adsorption process. This work suggests a promising approach for developing selective gas sensors capable of detecting weakly reducing gases.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
·Vol. 34
·期 44
·2405922
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IF 18.5
Minmin Ma,Ran Wang,Li Shi,Ronghua Li,Jie Huang,Zhuo Li,Peng Li,Elena Yu. Konysheva,Yanbo Li,Gang Liu,Xiaoxiang Xu
Photocatalytic carbon-carbon (C─C) coupling of benzyl alcohol is a promising means to coproduce the value-added chemicals with H 2 but is generally subject to low efficiency in terms of photon utilization. Here, efficient benzyl alcohol C─C coupling is achieved over Zn 2 In 2 S 5 containing a tunable content of Zn vacancies ( V Zn ). The V Zn tends to form shallow defect states below the conduction band that can expedite photocarrier separation by collecting the photo-generated electrons. The V Zn -collected electrons are essential for a high selectivity of the C─C coupling reactions because they enable a fast elimination of the byproduct benzaldehyde by catalyzing its reduction back to the ketyl radicals. Under simulated sunlight, the V Zn -containing Zn 2 In 2 S 5 accomplishes ≈100% conversion of benzyl alcohol for merely 1 h and attains ≈100% selectivity for the C─C coupling compounds for 2 h, delivering an apparent quantum yield as high as 7.7% at 420 ± 20 nm. The benefits of V Zn have also been verified by the theoretical calculations that indicate reduced energy barriers for various surface reactions in the presence of V Zn . This work brings fresh mechanistic insights into the role of V Zn and can serve as a useful guideline in the design of efficient photocatalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Chao Duan,Chun Tang,Yonghong Du,Shan Yu,Heng Guo,Yu Bai,Ying Zhou
Solar-driven electrochemical dissociation of hydrogen sulfide (H 2 S) to hydrogen and sulfur products in photovoltaic-electrochemical (PV-EC) devices becomes an effective strategy for acid gas purification and energy-saving hydrogen production . However, available H 2 S splitting electrochemical devices suffer from inferior energy conversion efficiency and fussy multi-step sulfur recovery problems. Herein, we propose an integrated solar-driven PV-EC system with diaphragm electrolytic reactor to solve these challenges. The optimized system integrated commercial silicon solar delivers a high solar-to-hydrogen energy conversion efficiency of up to 12 %, with approximately 99 % H 2 faradaic efficiency and demonstrates at least 50 hours of stability. More importantly, the S 2- /HS - can be transformed into add-valued Na 2 S 2 O 3 by one-step method in Na 2 SO 3 media, which avoids complex sulfur recovery. This work presents an alternative method of low-energy consumption for producing H 2 and high-value sulfur-related chemicals by H 2 S splitting through a PV-EC system.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Weijie Zhang,Shunshun Zhao,Yupeng Xing,Hongjie Qin,Qiling Zheng,Penghui Zhang,Shouwei Zhang,Xijin Xu
The sustainable conversion from solar energy to chemical energy is realized by using photocatalytic technology to produce hydrogen and hydrogen peroxide. In this work, the construction of a direct Z-scheme heterojunction is of great significance for improving the efficiency and stability of photocatalytic hydrogen evolution (PHE) and photocatalytic hydrogen peroxide production (PHP). In this study, P-doped h-BN (PBN) nanosheets are used to support the in-situ growth of ZnIn 2 S 4 nanoflowers via wet chemical method, and sandwich-like PBN/ZnIn 2 S 4 hierarchical heterostructures are successfully synthesized. The PHE performance of PBN/ZnIn 2 S 4 (∼59.46 μmol/h) is ∼ 2.35 times than that of the original ZnIn 2 S 4 (∼25.27 μmol/h), and the PHP performance (∼122.82 μmol/L/h) is 39.37 times than that of PBN (∼3.12 μmol/L/h). The excellent photocatalytic performance of PBN/ZnIn 2 S 4 can be attributed to the following points: (1) the acceleration of the separation of photogenerated electron-hole pairs induced by the formation of Z-scheme heterostructure; (2) reasonable design and construction of sandwich-like PBN/ZnIn 2 S 4 hierarchical heterostructure; (3) the promotion the migration and separation of photogenerated carriers by the built-in electric field. This work provides new ideas for the development of high-efficiency PHE and PHP Z-scheme heterojunction photocatalyst design.
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