Applied Sciences-Basel
·
2021
·Vol. 11
·期 22
·10854
·
IF 2.679
Jingyun Mao,Huiling Zhong,Xinpin Liu,Qingrong Qian,Yongjin Luo,Liren Xiao,Hun Xue
The development of a facile method for the synthesis of GaN:ZnO solid solution, an attractive material with a wurtzite-type structure, is vital to enhance its photocatalytic activity toward H2evolution. Herein, GaN:ZnO solid solution nanorods with diameters of around 180 nm were fabricated by combining the electro-spun method with a sequentially calcinating process. Photocatalytic water-splitting activities of the as-obtained samples loaded with Rh2−yCryO3co-catalyst were estimated by H2evolution under visible-light irradiation. The as-prepared GaN:ZnO nanorods at a nitridation temperature of 850 °C showed the optimal performance. Careful characterization of the GaN:ZnO solid solution nanorods indicated that the nitridation temperature is an important parameter affecting the photocatalytic performance, which is related to the specific surface area and the absorbable visible-light wavelength range. Finally, the mechanism of the GaN:ZnO solid solution nanorods was also investigated. The proposed synthesis strategy paves a new way to realize excellent activity and recyclability of GaN:ZnO solid solution nanorod photocatalysts for hydrogen generation.Keywords:GaN:ZnO solid solution nanorods;electrospinning technology;hydrogen evolution;visible-light photocatalysis
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Lili Deng,Ningjie Fang,Shilin Wu,Song Shu,Yinghao Chu,Jiaxiu Guo,Wanglai Cen
Constructing highly efficient and cost-effective photocatalyst system has been a big challenge for photocatalysis . Herein, CdS nanosphere ( N -CdS), hollow CdS (H-CdS) and a series of H-CdS@NiCoP core–shell nanospheres have been successfully prepared via a facile hydrothermal method . The activity test showed that H-CdS exhibited higher photocatalytic activity (3.34 mmol g -1 h −1 ) compared with N -CdS (0.99 mmol g -1 h −1 ) under visible light irradiation (λ ≥ 420 nm), suggesting that hollow structure could effectively improve photocatalytic activity. Moreover, the H-CdS@NiCoP-7 wt% displayed a maximum photocatalytic H 2 evolution rate of 13.47 mmol g -1 h −1 , which was about 4 times and 2.5 times higher than that of pristine H-CdS and H-CdS@Pt-3 wt%, respectively. Furthermore, H-CdS@NiCoP-7 wt% exhibited a good stability during 20 h test. The physicochemical properties were characterized by XRD , SEM , TEM, XPS , UV–vis DRS , PL and photoelectrochemical technique. The results showed that NiCoP addition can construct p-n junction with H-CdS and effectively promote the charge transfer from CdS to NiCoP, which improved the photocatalytic hydrogen evolution activity. This work revealed that NiCoP could react as an excellent co-catalyst for enhancing H-CdS photocatalytic activity.
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ACS Catalysis
·
2026
·
IF 13.6
Yang Pan,Zhou Xiaomei,Hou Yufeng,Guan Qingxin,Li Wei
Competitive H 2 oxidation severely limits CO 2 selectivity (typically <50%) during preferential CO oxidation (CO-PROX) on Pt catalysts. While metal–oxide interfaces can potentially circumvent this trade-off, constructing architectures that spatially decouple CO and H 2 activation remains challenging. Here, we report a junction-confined FeO-Pt/SiO 2 catalyst in which FeO species selectively decorate Pt nanoparticles, creating well-defined and closely contacted interfacial sites. Unlike randomly distributed FeO in conventional catalysts, this configuration enables electron redistribution from Pt to FeO, as revealed by Bader charge analysis. This electronic effect preserves strong CO adsorption on Pt (required for CO activation) while dramatically enhancing O 2 activation at the interface. Consequently, CO oxidation proceeds via a dominant low-barrier interfacial pathway (0.20 eV), while weakened H 2 adsorption at the FeO–Pt junction mitigates competitive H 2 oxidation under H 2 -rich conditions. The catalyst achieves >70% CO 2 selectivity at complete CO conversion over 80–160 ° C and maintains stability for 100 h without noticeable deactivation under H 2 -rich conditions. This work demonstrates that precise spatial organization of metal–oxide interfaces can effectively decouple competitive reaction pathways, offering a generalizable strategy for designing selective oxidation catalysts beyond CO-PROX.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Ping Bai,Junyu Lang,Song Wang,Haojie Tong,Wenling Du,Zhanli Chai
The elaborate modulation of charge transfer in Z-scheme heterojunctions is of significant importance yet poses a formidable challenge for achieving efficient photocatalytic hydrogen production . The present study reports the fabrication of ZnCdS nanoparticle wrapped by NiCo-layered double hydroxide with enriched oxygen vacancies (ZCS@LDH-O v ) was fabricated, which exhibits enhanced interfacial binding and internal electric field (IEF) in comparison to ZCS@LDH. Under visible-light irradiation, the as-prepared ZCS@LDH-O v exhibits a superior photocatalytic H 2 production rate of up to 2.68 mmol·g −1 ·h −1 , which is approximately 9.24-fold and 2.68-fold of the pristine ZnCdS and ZCS@LDH, respectively. The stability of the photocatalyst after 5 cycles is obviously enhanced, with ZCS@LDH exhibiting a remaining hydrogen evolution reaction (HER) rate of 52.7 % and ZCS@LDH-O v demonstrating an impressive remaining rate of 98.2 %. The Z-scheme facilitates rapid charge transfer and efficient separation, thereby enhancing the catalytic activity for HER. The excellent recyclability of ZCS@LDH-O v is primarily attributed to enhanced photo-corrosion resistance of ZnCdS, which can be ascribed to the efficient transfer of photo-generated holes through a rapid interfacial charge pathway.
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Molecular Catalysis
·
2023
·
IF 4.6
Qiaona Liu,Xin Han,An Qian,Xin Pu,Lei Ye,Pengpeng Liu,Fengqi Zhang,Jichang Liu
Developing noble-metal-free dual-metal single-atom catalysts with rich active accessible sites and excellent catalytic activity is very meaningful and challenging, especially for photocatalytic hydrogen production reaction, which can significantly reduce the cost of photocatalytic technology application while reducing the use of noble metals. Herein, a novel noble-metal-free dual CuNi single-atom modified ZnIn 2 S 4 (CuNi SA -ZIS) photocatalyst with high hydrogen production performance were successfully prepared by a hydrothermal method. The ZnIn 2 S 4 with a spherical nanoflower structure is composed of ultrathin nanosheets, and AC HDDAF-STEM results shows that CuNi bimetallic particles are uniformly distributed on the surface of ZnIn 2 S 4 nanosheets and exhibit atomic level dispersion, forming dual-metal single-atom structure. The optimized 1 wt% CuNi SA -ZIS photocatalyst with the Cu/Ni ratio of 1:1 shows the optimum H 2 evolution performance with a rate of up to 7844.7 μmol· g −1 · h −1 using triethanolamine as a sacrificial reagent, which is significantly improved compared to pristine ZIS, Cu-ZIS and Ni-ZIS samples under simulated sunlight. Electrochemical and spectroscopic characterization results demonstrated that the improved photocatalytic activity of CuNi SA -ZIS was mainly due to the addition of the dual CuNi single atoms with a synergistic effect served as a co-catalyst for ZnIn 2 S 4 photocatalysts, providing efficient active sites for hydrogen evolution while preventing the fast recombination of photo-generated electrons and holes. This study provides a valuable source of ideas for the design of effective noble-metal-free dual-metal single-atom catalysts.
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CHINESE JOURNAL OF CATALYSIS
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2023
·
IF 16.5
Xiao-Juan Li,Ming-Yu Qi,Jing-Yu Li,Chang-Long Tan,Zi-Rong Tang,Yi-Jun Xu
The simultaneous utilization of photogenerated electrons and holes in one cooperative photoredox system for the dehydrocoupling of thiols into value-added disulfides and clean hydrogen (H 2 ) fuel meets the development criteria of green chemistry. Herein, we report the synthesis and application of cocatalyst PdS decorated ZnIn 2 S 4 (PdS-ZIS) composites for photocatalytic coupling of thiols into disulfides and H 2 evolution under visible light irradiation. The superior photocatalytic performance over PdS-ZIS composites compared with blank ZIS is attributed to the function of PdS as oxidation cocatalyst, which dramatically promotes the separation and transfer of photogenerated charge carriers due to its excellent hole trapping ability. In-situ Fourier transform infrared spectra reveal the dynamic variation of reactants on the catalyst surface. Electron paramagnetic resonance technology confirms that sulfur-centered radicals are the key reaction intermediates in this coupling process. Moreover, the application of PdS-ZIS composites to the dehydrocoupling of various thiols with different substituent groups into the corresponding S–S coupling products has been demonstrated to be practicable. This work is expected to offer insights into the rational design of cocatalyst-decorated semiconductor photocatalysts with efficient utilization of photogenerated electrons and holes for the co-production of high-value chemicals and clean H 2 energy in a cooperative photoredox catalysis process.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
·
IF 7.2
Yuwen Tian,Yuanzhi Hong,Bingqi Chen,Kun Zhang,Dunhua Hong,Xue Lin,Junyou Shi
Indium oxide (In 2 O 3 ) is a promising semiconductor used for various photocatalytic reactions, yet the green and template-free synthesizing the different micro/nanostructured In 2 O 3 with tunable morphology is still full of challenge. In this study, the three morphological In 2 O 3 with 3D micro-cubelike (In 2 O 3 -MC), 3D micro-ricelike (In 2 O 3 -MR), and 2D nano-platelike (In 2 O 3 -NP) were successfully fabricated through a facile hydrothermal strategy without any organic template additives. Owing to the enlarged specific surface area , promoted charge migration rate and suitable surface oxygen vacancies density, the unique 3D ricelike In 2 O 3 -MR exhibited the best photocatalytic H 2 generation activity from biomass glucose solution, which was 1.9-fold and 1.7-fold higher than that of In 2 O 3 -MC and In 2 O 3 -NP under the same experimental conditions. In addition, the optimum photoactivity of In 2 O 3 -MR was achieved under the alkaline environment with pH = 11 and 1.0 wt% Pt cocatalyst loading, which was better than the most of previously reported In 2 O 3 -based photocatalysts . Simultaneously, the possible photocatalytic mechanism for solar H 2 evolution from glucose solution was also discussed. Our work will bring about potential application in preparation of other photocatalysts with controlling morphology for renewable photocatalysis .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Li Li,Kaixuan Kuang,Xiuzhen Zheng,Jiahui Wang,Wei Ren,Jingbiao Ge,Sujuan Zhang,Shifu Chen
To enhance the efficiency of photocatalytic H 2 evolution, numerous methods are employed by increasing the utilization of photogenerated charge carriers (PCCs), including catalyst design, defect regulation, and selection of suitable H + resources. Using self-assembly method, CoWO 4 /Zn x Cd 1−x S with p–n heterojunction was synthesized. Although CoWO 4 (CW) cannot produce H 2 under visible light irradiation, it can provide photogenerated electrons (e − ) to Zn 0.3 Cd 0.7 S (ZCS), and largely increase the photocatalytic activity of ZCS. The optimal CW/ZCS composite can reach 15.58 mmol·g −1 ·h −1 , which is 45.8 and 24.3 times higher than the values of the pure CdS and ZCS, respectively. The largely enhanced photocatalytic H 2 production is attributed to the Zn vacancies (V Zn ), p–n heterojunction, and p-chlorobenzyl alcohol (Cl–PhCH 2 OH) as the H + source of H 2 production. V Zn on the ZCS surface as the capture center of photogenerated holes (h + ), can regulate the carrier distribution, which results in more photogenerated e − and less generated h + . The combination of p–n heterojunction and V Zn can enhance the separation and transfer efficiency of PCCs, and effectively inhibit the recombination of charge carriers. To further improve the utilization rate of PCCs, the photocatalytic H 2 evolution is proceeded by Cl–PhCH 2 OH oxidation in N , N -dimethylformamide solution, with 4-chlorobenzaldehyde (Cl–PhCHO) generated. The separated photogenerated e − and h + both participated in the redox reaction of H + reduction and Cl–PhCH 2 OH oxidation, considering that the amount of H 2 and Cl–PhCHO products are close to 1:1. This work not only facilitates the separation and transfer of PCCs, but also provides directions for the design of efficient photocatalysts and H 2 evolution in the organic phase.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Yanlin Jia,Zizhao Wang,Xiu-Qing Qiao,Lei Huang,Shenglong Gan,Dongfang Hou,Dong-Sheng Li
Metallic MoSe 2 with distinct platinum-like electronic configuration and compelling band gap structure exhibits zero approaching Gibbs free energy for H atom, hence can be approved as an ideal cocatalysts for H 2 evolution. However, the reports on MoSe 2 cocatalyst still leaves much room. Here, two dimensional ultrathin MoSe 2 nanosheets bedecked Zn 0.5 Cd 0.5 S nanoparticles were reported as efficient photocatalyst, in which metallic MoSe 2 nanosheets cocatalyst will do duty for electron sink to promote the separation of charge carriers and prolong the electrons lifetime, thus benefiting the improved photocatalytic H 2 evolution activity. As a result, Zn 0.5 Cd 0.5 S/MoSe 2 composite with an optimized 9 wt% MoSe 2 presents a higher H 2 evolution activity of 4853.3 μmol g -1 h −1 , 3.57 folds of pure Zn 0.5 Cd 0.5 S sample (1361.0 μmol g -1 h −1 ). Meanwhile, the greatly enhanced photo-reduction efficiency for toxic heavy metal Cr (VI) ion by Zn 0.5 Cd 0.5 S/MoSe 2 composite further certifies the promoted separation of electron- hole pairs. These results turned out that MoSe 2 is qualitied as candidate to serve as promising co-catalyst for photocatalyst energy conversion and decontamination.
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MATERIALS LETTERS
·
2021
·
IF 3.423
Tianming Zhao,Qi Wang,An Du
To alleviate the energy shortage and to improve the environmental problems, low-cost and highly efficient materials for H 2 production are of considerable importance. Here, we report a nanostructure from CuS/ZnO NWs on steel mesh via a two-step hydrothermal route for piezo-photocatalytic H 2 production. The CuS/ZnO exhibits an absorption band in visible and ultra-violet bands. Under solar and ultrasonic exposure, the CuS/ZnO NWs demonstrate great piezo-photocatalytic performance (140 μmol g −1 h −1 ). The working mechanism can be attributed to the piezo-photocatalytic effect that the photogenerated electrons and holes are driven along opposite directions by built-in electrical field, decreasing the recombination rate and producing H 2 . This H 2 production mechanism holds great promise for development novel clean fuel.
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CATALYSIS LETTERS
·
2021
·Vol. 152
·期 2
·610-618
·
IF 3.186
Zhou Junjie,Yan Jiaying,Meng Xu,Chen Weifeng,Guo Jianfeng,Liu Xiang
Abstract It is still a significant challenge to replace noble metal based catalysts by non-noble metal-based, highly efficient and earth-abundant catalysts in the H 2 generation upon hydrolysis of sodium borohydride. Herein, we first design and synthesize the highly selective and heterogeneous Co x W y nanocomposites from ZIF-67 as robust catalysts for H 2 production upon the hydrolysis of sodium borohydride. Among them, the Co 0.45 W 0.55 nanocatalyst exhibits the highest TOF of 1770 mL H2 g cat −1 min −1 (the TOF related to only cobalt nanoparticles 8401 mL H2 g Co −1 min −1 ) over pure ZIF-67 or W nanoparticles and other ones. In addition, the Co 0.45 W 0.55 catalyst has been successfully recycled at least 5 times without any significant activity loss, although the W (VI) has been partly reduced to W (V), W (IV) and W (0) in the hydrolysis of sodium borohydride. This stability is taken into account by the highly active Co species rather than the activity of W itself. Based on the results obtained, we have shown that Co 0.45 W 0.55 nanocomposite can be a potential candidate for the replacement of a noble metal catalyst for H 2 generation. Graphic Abstract
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Di Li,Yiming Huang,Zengyong Li,Linxin Zhong,Chuanfu Liu,Xinwen Peng
The electrocatalytic water splitting for hydrogen production is greatly limited by the sluggish anodic OER. Herein, a hybrid of cobalt nanoparticles supported in nitrogen doped porous carbon (Co@NPC) is prepared by using a biomass-based ternary deep eutectic solvent (DES) as precursor and self-templates, which is utlized as bifunctional electrocatalyst for boosting H 2 generation and converting glucose into valuable chemicals simultaneously. Importantly, only a small cell voltage of 1.56 V is required to deliver 10 mA cm −2 , which is 180 mV lower than that of overall water splitting. Density functional theory (DFT) calculations confirm that nitrogen doping porous carbon could synergistically optimize adsorption energies of H 2 O (ΔE *H2O ) and *H adsorption free energies (ΔG *H ), enhancing catalytic activity toward HER. This work highlights the potential application prospects of using glucose oxidation reaction (GOR) instead of OER to promote H 2 generation and product value-added chemicals.
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