Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 10
·4485-4493
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IF 9.931
Lingyou Zeng,Kaian Sun,Zhichao Yang,Shengli Xie,Yanju Chen,Zhi Liu,Yaqing Liu,Jinchong Zhao,Yunqi Liu,Chenguang Liu
Three-dimensional (3D) nanomaterials have received significant attention for large-scale functional applications due to their large specific surface areas as well as desired electrical, physicochemical, and catalytic properties. Herein, we present a facile and effective synthetic route for in situ grown 3D hierarchical Ni3S2 superstructures (rod-like arrays and nanoforest patterns) on nickel foam. This handy strategy endows the Ni3S2 superstructures with large surface active areas, porosity, and macro-/mesoporous structures. We have shown that these materials can serve as highly active, binder-free, bifunctional electrocatalysts for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Moreover, these materials were found to provide a ∼100% faradaic yield towards both HER and OER and exhibit remarkable catalytic stability (for >50 h).
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WASTE MANAGEMENT
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2024
·
IF 7.1
Pengpeng Luan,Tiecheng Liu,Jinglan Wang,Beibei Yan,Guanyi Chen,Zhanjun Cheng
In this study, ex-situ catalytic pyrolysis of oxygen-containing polycarbonate (PC) was conducted to prepare carbon nanotubes (CNTs) and H 2 -rich syngas. This study examined the influence of the active metal components (Ni and Fe), catalyst pre-reduction, and pre-deoxygenation of pyrolysis volatiles on the catalytic performance and mechanism. Results show that the reductive constituents in pyrolysis volatiles make it difficult to reduce the Fe oxides, thus hindering the CNTs growth on Fe catalysts, compared to Ni catalysts. H 2 pre-reduction of Ni and Fe catalysts enhances the generation of CNTs and syngas. The pre-reduced Fe catalyst exhibits better carbon deposit performance, reaching 263 mg/g plastics . The pre-reduced Ni catalyst better facilitates the reforming reaction of CO 2 and H 2 O, resulting in higher syngas yields of 32.75 mmol/g plastics , with a volume proportion of 94.4 vol%. The addition of the deoxygenation catalyst Ni/HZSM-5 promotes the growth of CNTs with fewer defects and higher graphitization on Ni catalysts. The excess CO 2 and H 2 O generated by the introduction of Ni/HZSM-5 may oxidize the Fe 0 on pre-reduced Fe catalysts, inhibiting the growth of CNTs. The mechanism of the growth of CNTs and syngas from PC is also explored. The findings can provide theoretical guidance for the disposal of waste plastics.
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Journal of Environmental Chemical Engineering
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2024
·
IF 7.4
Chuanhao Li,Yi Tian,Shuangyu Wang,Ping Yang,Xiao Zhang
To improve the stability of Ag based co-catalysts and to increase the photocatalytic performance of graphitic carbon nitride (g-C 3 N 4 ), Ag 2 Se nanoparticles were grown onto superior thin sulfur-doped g-C 3 N 4 nanosheets which was fabricated via two-step thermal polymerization at high temperature. Ultrathin S-doped g-C 3 N 4 nanosheets were prepared via two-step thermal polymerization using melamine and thiourea. The ratios of Ag 2 Se were adjusted to fabricate a series of Ag 2 Se/S-g-C 3 N 4 (Ag 2 Se/SCN) composite samples by controlled solvothermal synthesis. S-doping plays an important role in mono-dispersion of Ag 2 Se nanoparticles on S-g-C 3 N 4 nanosheets because of the control of growth sites. The photocatalytic removal of tetracycline hydrochloride test indicates that sample Ag 2 Se/SCN-3 with Ag 2 Se loading of 3 % reveals the best removal effect, in which tetracycline hydrochloride of 60 % is removed within 60 min. Photocatalytic hydrogen generation test results without co-catalyst addition demonstrate that sample Ag 2 Se/SCN-3 exhibits the best H 2 evolution rate of 2116.35 μmol·g −1 ·h −1 , which is 3.8 times of that of pure carbon nitride. The photocatalytic mechanism tests suggest that Schottky heterojunctions are formed in the Ag 2 Se/S-g-C 3 N 4 composites. The formation of Schottky heterojunctions improved the separation efficiency of photogenerated charge carriers. The incorporation of Ag 2 Se nanoparticles (as the co-catalyst) on S-g-C 3 N 4 nanosheets is the key for drastically improving the photocatalytic performance and eliminating the use of Pt co-catalyst during the photocatalytic processes.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
·
IF 14.7
Wan Sijie,Wang Wang,Cheng Bei,Luo Guoqiang,Shen Qiang,Yu Jiaguo,Zhang Jianjun,Cao Shaowen,Zhang Lianmeng
The rapid recombination of photoinduced charge carriers in semiconductors fundamentally limits their application in photocatalysis. Herein, we report that a superlattice interface and S-scheme heterojunction based on Mn 0.5 Cd 0.5 S nanorods can significantly promote ultrafast charge separation and transfer. Specifically, the axially distributed zinc blende/wurtzite superlattice interfaces in Mn 0.5 Cd 0.5 S nanorods can redistribute photoinduced charge carriers more effectively when boosted by homogeneous internal electric fields and promotes bulk separation. Accordingly, S-scheme heterojunctions between the Mn 0.5 Cd 0.5 S nanorods and MnWO 4 nanoparticles can further accelerate the surface separation of charge carriers via a heterogeneous internal electric field. Subsequent capture of the photoelectrons by adsorbed H 2 O is as fast as several picoseconds which results in a photocatalytic H 2 evolution rate of 54.4 mmol·g −1 ·h −1 without any cocatalyst under simulated solar irradiation. The yields are increased by a factor of ~5 times relative to control samples and an apparent quantum efficiency of 63.1% at 420 nm is measured. This work provides a protocol for designing synergistic interface structure for efficient photocatalysis.
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CRYSTENGCOMM
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2024
·Vol. 26
·期 38
·5440-5451
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IF 2.6
Xiaoyun Ye,Hangyu Zhong,Yumei Zhang,Xuehua Liu,Wei Tian,Li-An Ma,Qianting Wang
Previous studies on photocatalytic technology have shown that doping co-catalysts and constructing composite heterojunctions are effective strategies for improving the photocatalyst performance. The Ti3C2/SrTiO3/g-C3N4 composite photocatalyst with a gradient heterostructure was prepared by the high-temperature calcination method with Ti3C2 as the co-catalyst. The effects of g-C3N4 content on the microstructure and hydrogen evolution rate of the Ti3C2/SrTiO3/g-C3N4 composites were investigated under simulated sunlight. The results showed that the photocatalyst with 60 wt% of g-C3N4 had the optimal hydrogen evolution rate of 1733.13 μmol g−1 h−1 after simulated sunlight irradiation for 4 h, which was approximately 3.3 times higher than that of Ti3C2/SrTiO3. After four photocatalytic hydrogen evolution cycles, no significant decrease in the hydrogen evolution rate of the Ti3C2/SrTiO3/g-C3N4 composite was observed. This work may serve as a rational reference on the synergistic effect of heterostructures and cocatalysts to improve the separation effect of electron–hole pairs, thus improving the hydrogen evolution effect of the catalyst.
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ENERGY & FUELS
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2024
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IF 5.2
Jinbo Yang,Shengqi Lin,Chunhe Li,Kuankuan Ren,Qiufeng Ye,Weidong Dou
Utilizing photocatalytic technology to efficiently convert biomass-derived compounds into value-added chemicals and release hydrogen gas can effectively address energy and environmental issues. For this purpose, we fabricated a series of NiMoS4/Zn0.6Cd0.4S nanocomposites through a simple two-pot hydrothermal treatment. Dexterously, the photoexcited electrons and holes can be simultaneously utilized to participate in a photocatalytic redox reaction, effectively achieving the oxidation of furfuryl alcohol while cooperating with H2 evolution. The hydrogen evolution rate of 10%-NiMoS4/Zn0.6Cd0.4S nanocomposite in 1.50 vol % furfuryl alcohol aqueous solution is as high as 289.5 μmol·h–1, which is approximately 2895 and 41 times higher than that of pure NiMoS4 and Zn0.6Cd0.4S, respectively. Meanwhile, after 13 cycles of photocatalytic reaction, the conversion efficiency and selectivity of converting furfuryl alcohol to furfural are 68.5% and 94.0%, respectively. This photocatalyst also shows high photocurrent, low impedance, and efficient photogenerated carrier separation and transport properties, which can be attributed to the establishment of an ohmic junction between NiMoS4 and Zn0.6Cd0.4S. It is anticipated that this work can provide inspiration for the effective conversion of biomass-derived platform chemicals into high-value chemicals through visible-light-driven photocatalytic technology.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Jing Wang,Xingyu Niu,Qi Hao,Kun Zhang,Xinyi Shi,Liping Yang,Hui Ying Yang,Jilei Ye,Yuping Wu
Low charge separation efficiency significantly hampers the performance of photocatalytic hydrogen production. Constructing heterojunctions emerges as a crucial strategy to enhance photocatalytic activity by improving charge separation. An S-scheme heterojunction not only effectively separates the photogenerated charge in composite photocatalysts but also preserves optimal redox capabilities. This study presents the first report of CuInS 2 /CeO 2 (CIS/CeO 2 ) and demonstrates how charge separation within CIS/CeO 2 to enhance photocatalytic hydrogen production through the construction of an S-scheme heterojunction. The UV–visible-driven hydrogen production rate of CIS/CeO 2 is 4.6 and 9.4 times higher than that of CIS and CeO 2 alone, respectively. The improved photocatalytic performance primarily stems from enhanced charge separation promoted by the S-scheme heterojunction. The charge transfer pathway was confirmed as an S-scheme mechanism through a combination of band structure experiments, density functional theory (DFT) calculations on work function, internal electric field, and charge differential density distribution, alongside electron paramagnetic resonance (EPR) experiments. Multiple perspectives were employed to elucidate the reasons behind facilitating efficient charge separation. This research provides valuable insights for advancing photocatalytic performance.
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SENSORS AND ACTUATORS B-CHEMICAL
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2024
·
IF 8
Jiamin Li,Shenghong Li,Shihao Lu,Xuhui Geng,Yafeng Guan
A micron-scale bilayer sensor was fabricated in situ by electrohydrodynamic jet printing for detecting H 2 gas with highly selectivity, sensitivity and stability. The sensor consisted of a Pt loaded mesocellular silica foam (Pt-MCF) catalytic filter layer, and a ZnO/SnO 2 /Au (ZSA) sensing layer. Benefiting from the selective catalytic oxidation for CO in the catalytic filter layer, the cross-interference of CO on this sensor was reduced from 58 % to 15 %. The sensor also demonstrated a satisfactory selectivity to H 2 in interfering gases of CO 2 and CH 4 due to its high specific response to H 2 . In the ZSA sensing layer, the n-n heterojunction (ZnO-SnO 2 ) and abundant active sites on the Undaria pinnitafida -like curved nanosheet structure effectively enhanced the response of H 2 by 6.7 times. The sensors exhibited a wide H 2 dynamic range of 0.5–500 ppm with low detection limit of 94 ppb. The response/recovery time to 50 ppm H 2 was 24 s/35 s. The sensor also showed good long-term stability in 28-day response-repeatability measurement (RSD=5.3 %) and good anti-humidity.
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FUEL
·
2025
·
IF 7.5
Zhangkai Qian,Jia-qi Bai,Mei Ma,Huangfei Liu,Mengdie Cai,Jingshuai Chen,Song Sun
N -methylation of amines, nitro compounds and nitriles with CO 2 and H 2 offers a promising strategy for CO 2 utilization. However, developing highly efficient and stable Cu-based catalysts for selective mono- N -methylation of aniline remains challenging. Herein, we report the successful synthesis of a Cu-ZnO/TiO 2 catalyst, with the optimized 5 %Cu-7.5 %ZnO/TiO 2 catalyst achieving a 96.7 % yield of N -methylaniline (MA) and an initial turnover frequency (TOF) of 7.4 h −1 after 6 h under 453 K, 2 MPa CO 2 and 4 MPa H 2 . This performance surpasses all reported Cu-based catalysts and rivals noble metal-based systems. The catalyst demonstrated reusability at least four cycles and versatility in the N -methylation of various amines, nitro compounds, and nitriles. Kinetic studies revealed reaction orders of 0 with respect to aniline concentration and CO 2 pressure, and 1 with respect to H 2 pressure. Based on kinetics and extensive characterization, we propose a reaction mechanism over 5 %Cu-7.5 %ZnO/TiO 2 , identifying Cu nanoparticles as the active sites. The process proceeds via N -phenylcarbamic acid and N -phenylformamide intermediates, with the hydrogenation of N -phenylcarbamic acid as the rate-determining step.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2025
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IF 2.9
Qianqian Peng,Chengxuan Zhou,Shucan Qin,Jinbiao Liang,Shengyun Xu,Jiaming Mao,Jianming Shi,Yanrong Liu,Yunqian Ma
Electrochemistry allows for the simultaneous conversion of hydrogen sulfide (H2S) to hydrogen (H2) and sulfur, achieving atomic economy, and is a sustainable and cost-effective method. At the same time, an electrolyte with high conductivity and H2S absorption that can effectively capture H2S in an electrochemical process is essential. An ionic liquid electrolyte system for the absorption and electrolysis of H2S was constructed using the guanidine salt ionic liquid with amine-based functional groups as the carrier electrolyte, water as the solvent, and NaOH as the H2S absorber. The prepared electrolyte ([TMG][IM]-AE-30) showed a strong absorption of H2S with an equilibrium solubility of 100.82 g L−1. Under constant potential electrolysis at 1.0 V vs. RHE, the maximum hydrogen production rate reaches 2919.97 μmol h−1 and the Faraday efficiency reaches 99%, and the anodic product is α-sulfur with a production of 0.881 g after electrolysis for 8 h; the current density and hydrogen production rate are still higher than those of the AE systems after three cycles. Overall, the system has good hydrogen sulfide absorption and electrolysis performances, and [TMG][IM] can effectively improve the H2S absorption and electrolysis efficiencies.
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CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Eryu Wang,Yi-Chun Chu,Wenjun Zhang,Yanping Wei,Chuanling Si,Regina Palkovits,Xin-Ping Wu,Zupeng Chen
The co-production of hydrogen and value-added biochemicals from lignocellulose utilizing solar energy has been regarded as one of the technologies most potentially able to alleviate the current energy crisis. Here, we demonstrate a cost-effective photoreforming strategy for lignocellulose valorization using a carbon nitride-supported platinum single-atom photocatalyst. An advanced H 2 evolution rate of 6.34 mmol mol Pt –1 h –1 is achieved over the optimal catalyst, which is around 4.6 and 30.5 times higher compared with the nanosized Pt counterpart and pristine carbon nitride, respectively. Meanwhile, the monosaccharides are oxidized to value-added lactic acid with >99% conversion and extraordinary selectivity up to 97%. The theoretical calculations show that with Pt incorporation, the photogenerated holes are predominantly localized on the metal sites while the photogenerated electrons are concentrated on C 3 N 4 , thus enhancing the effective separation of charge carriers. This work provides a promising avenue for the simultaneous production of green H 2 and bio-based chemicals by biomass photorefinery.
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Journal of Energy Chemistry
·
2025
·
IF 14.9
Ali Hammad,Siyi Zou,Fandi Ning,Ghulam Nabi,Yuzhuo Jiang,Bin Tian,Wentao Huang,Muhammad Rashid,Shiqi Zhao,Xiaochun Zhou
Inorganic materials can solve transportable and on-site hydrolytic hydrogen generation issues. CaH 2 /(Al/Si) composites are preferable due to their notable chemical properties. However, these composites require pretreatments, an inert environment, and long hours of physical ball milling for high homogeneity and synergistic effects. CaH 2 also inhibits the hydrolysis reaction by forming its products on the Al/Si surface, which hinders the direct utilization of composites. This work represents the first investigation of NaH-CaH 2 (Al/Si) fuel composites, which greatly overcome these limitations and can be directly used for on-site hydrogen generation and proton exchange membrane (PEM) fuel cells. The NaH-CaH 2 (Al/Si) fuel composites were prepared by using a straightforward mixing method with variable composition ratios, showing high H 2 yield and fuel cell (FC) performance. NaH addition provides the bridge effect, which opens up a new way to enable efficient hydrolysis and greatly enhances the hydrolysis activity of CaH 2 /(Al/Si) composites. The novel fuel composites (NaH-CaH 2 /Al) have extraordinary FC performance and a 0.42 W/cm 2 peak power density greater than commercial hydrogen generators. It provides high H 2 yield 84.4 % for NaH-CaH 2 /Al and 82 % for NaH-CaH 2 /Si compared to NaOH-CaH 2 (Al/Si), NaCl-CaH 2 (Al/Si), and KCl-CaH 2 (Al/Si) composites. The NaH bridge effect hinders the direct water contact and stops the formation of Ca(OH) 2 around Al/Si, which provides adequate pathways for the CaH 2 (Al/Si) hydrolysis. The impressive capabilities of novel fuel composites are anticipated to offer practical uses in fuel cells, automobile applications, and portable/on-board H 2 generation.
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