CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Zhuogen Li,Gangqiang Zhu,Weibin Zhang,Lujun Zhu,Baowei Cao,Jianzhi Gao,Xianjin Shi,Yu Huang,Peng Liu,Mirabbos Hojamberdiev
In recent years, metal–semiconductor heterojunctions have been intensively researched in the field of photocatalysis due to the effective spatial separation of photo-induced electron-hole pairs. Here, the dual-functional copper (Cu 0 /Cu 2+ )-modified SrTiO 3-δ nanosheets (Cu/STCO) are successfully synthesized by a two-step route. First, Cu 2+ -doped SrTiO 3-δ (STCO) nanosheets are synthesized by a hydrothermal method and then Cu 0 nanoparticles (NPs) are in situ formed from the STCO under H 2 atmosphere at 500 °C. The optimized ratio 6 %-Cu/STCO photocatalyst exhibits the best photothermal catalytic performance for CO 2 reduction reaction (CO 2 RR) and H 2 evolution performance. The detailed characterization demonstrate that the Cu 2+ dopant extend the light absorption range and the in situ generated Cu 0 NPs effectively improve the separation ability of photogenerated charge carriers by forming the Schottky contact with STCO. The excited localized surface plasmon resonance (LSPR) effect of metallic Cu 0 in Cu/STCO shows a considerable catalysis performance even under 600 nm monochromatic light irradiation. The density functional theory (DFT) calculations suggest that the Cu/STCO diminishes the barrier of the rate-determining steps of the CO 2 RR and H 2 evolution thus perform the outstanding catalysis ability in two filed. This work presents the synergistic effect of Cu 0 and Cu 2+ on enhancing the photothermal catalytic performance for CO 2 RR and H 2 evolution and offers a novel strategy to synthesize the metal–semiconductor nanostructures for efficient harnessing of solar energy into fuel.
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高影响因子
Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 48
·33640-33648
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IF 10.7
Junli Chen,Xinyi Jin,Xinli Yang,Lei Deng,Zhiqiang Zhang,Lifeng Han,Feilong Gong,Yonghui Zhang
Ultrathin Mo-HNb3O8 nanosheets were synthesized by a facile hydrothermal process. Introducing low-valence Mo and oxygen vacancies into the pristine HNb3O8 nanosheets can modulate the band structure and induce the localized surface plasmon resonance (LSPR) to increase the charge-carrier densities and produce hot carriers derived from the non-radiative decay of LSPR, which not only efficiently promotes the separation and transfer of photo-generated carriers, but also improves the high utilization rate of solar energy in photothermal catalytic hydrogen evolution in the full solar spectrum. The optimized MoNb-10 exhibits the highest H2 evolution rate (220.4 μmol h−1 g−1), which is approximately 7.7 times higher than that of the HNb3O8 nanosheet. The current work not only deepens our understanding of LSPR effects generated from the Mo dopant and OVs on the surface of transition metal oxide nanosheets, but also provides clues for exploring new photothermal catalysts to promote future solar energy conversion.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Jiejie Bai,Yue Shi,Aixin Ma,Feifei Liu,Yanru Liu,Caixia Li,Jianping Lai,Lei Wang
The production of three separated, high-value chemicals (H 2 O 2 , urea and H 2 ) from CO 2 , N 2 , and H 2 O represents a significant challenge. It is a prospective and innovative way to simultaneously produce these chemicals in an anion exchange membrane (AEM) electrolyzer, which couples anodic 2e - water oxidation (2e - WOR) and cathodic CO 2 , N 2 and water reduction reaction (CNWRR), but has not yet been realized. Here, we found that bifunctional Cu x Ti 1-x O 2-y catalysts can be employed in the electrochemical production of H 2 O 2 , urea and H 2 from CO 2 , N 2 and water, and the optimized Cu 0.12 Ti 0.88 O 2-y catalyst exhibits an excellent productivity of 11.8 μmol cm −2 min −1 , 0.3 mg cm -2 h −1 and 0.82 mmol cm -2 h −1 for H 2 O 2 , urea and H 2 at 4.0 V (50 mA cm −2 ) in AEM electrolyzer, respectively. Theoretical calculations reveal that the superior performance of the 2e - WOR and CNWRR is attributed to the Cu doping effect, which not only promotes the coupling of *OH but also optimizes the adsorption energy barriers of COOH* and NNH*. It is worth noting that the AEM electrolyzer assembled by bifunctional Cu 0.12 Ti 0.88 O 2-y reaches a current density of 50 mA cm −2 with a cell voltage of 4.0 V and exhibits excellent stability of 50-hour continuous operation.
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ChemSusChem
·
2024
·
IF 7.5
Weikang Wang,Shaobin Mei,Shahid Khan,Yujue Hu,Lijuan Sun,Muhammad Adnan Qaiser,Chengzhang Zhu,Lele Wang,Qinqin Liu
Graphical A molecular-level hierarchical Znln 2 S 4 /HPW S-scheme heterojunction was prepared through one-pot hydrothermal method in this work. The obtained Znln 2 S 4 /HPW heterojunction photocatalysts indicated molecular-level interfacial contact, enhanced light absorption, and accelerated charge separation and transfer, achieving efficient overall H 2 production and benzyl alcohol oxidation with corresponding photogenerated electrons and holes, respectively. Simultaneous utilization of photogenerated electrons and holes to achieve overall redox reactions is attractive but still far from practical application. The emerging step (S)-scheme mechanism has proven to be an ideal approach to inhibit charge recombination and supply photoinduced charges with highest redox potentials. Herein, a hierarchical phosphotungstic acid (H 3 PW 12 O 40 , HPW)@Znln 2 S 4 (ZISW) heterojunction was prepared through one-pot hydrothermal method for simultaneous hydrogen (H 2 ) evolution and benzyl alcohol upgrading. The fabricated HPW-based heterojunctions indicated much enhanced visible-light absorption, promoted photogenerated charge transfer and inhibited charge recombination, owing to hierarchical architecture based on visible-light responsive Znln 2 S 4 microspheres, and S-scheme charge transfer pathway. The S-scheme mechanism was further verified by free-radical trapping electron spin resonance (ESR) spectra. Moreover, the wettability of composite heterojunction was improved by the modification of hydrophilic HPW, contributing to gaining active hydrogen (H + ) from water sustainably. The optimal ZISW-30 heterojunction photocatalyst indicated an enhanced hydrogen evolution rate of 27.59 mmol g −1 h −1 in benzyl alcohol (10 vol. %) solution under full-spectrum irradiation, along with highest benzaldehyde production rate is 8.32 mmol g −1 h −1 . This work provides a promising guideline for incorporating HPW into S-scheme heterojunctions to achieve efficient overall redox reactions.
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PubMed
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Junwen Cai,Xin Jiang,Linfeng Zhang,Benoit Couturaud,Wen-Zhuo Tang,Yao-Yan Zhang,Rui-Bo Jin,Yoann de Rancourt de Mimérand,Xiaoyun Jin,Jia Guo
A multifunctional, multiphase-supported photocatalyst was fabricated via the combination of LCD three-dimensional (3D) printing, cold plasma discharge (CPD) technology, and surface chemistry to be used for the degradation of organic pollutants in water and for the generation of hydrogen gas. BiOBr was chosen as the main catalytic phase and was used in association with a phosphor, SrAl2O4:Eu2+,Dy3+ (SAED), and a metal–organic framework, Ni-BDC. Their immobilization was realized thanks to polydopamine (PDA), which is used as a coupling agent. While BiOBr was the most active photocatalytic phase, the phosphor acted as a light-storing component for photodegradation in the dark and overall, as a boost for photoactivity. PDA also boosted the photoactivity, in parallel with its crucial role in the immobilization of the SAED/Ni-MOF/BiOBr catalyst on fractal polymer support. An in situ complexation-assisted precipitation (ISCAP) process was used, allowing the formation of the catalytic phases with nano features. The resulting hybrid photocatalysts were tested through rhodamine B (RhB) dye photodegradation upon visible light irradiation or light/dark alternating conditions to simulate more realistic variable light illumination. We found that, although used in a very small amount, the Ni-MOF had a significant impact on the photoactivity, forming a Z-scheme heterojunction with BiOBr. Finally, H2 evolution testing further established the photocatalytic activity and versatility of the supported catalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Xiaolin Guo,Wangxiang Ye,Zi’ang Chen,Ang Zhou,Dingfeng Jin,Tingli Ma
Aiming for purification the trace amount of CO in H 2 -rich streams with reduced energy consumption and low cost, solar-driven photothermal preferential oxidation of carbon monoxide on the non-precious metal oxide catalyst is proposed in this work. Cu doped CuCeO 2−x nanorods catalysts were synthesized with a fast and simple coprecipitation method at the room temperature , which shows high CO oxidation activity in photothermal preferential oxidation of CO (CO-PROX) under UV-Vis-IR light irradiation . Rely on the various characterization methods such as UV-Vis-IR diffuse reflection spectrum (UV-Vis-IR DRS), photoluminescence spectrum (PL), transient photocurrent test, HRTEM , XRD , XPS, UV-Raman and H 2 -TPR, the optical and chemical properties of the CuCeO 2−x nanorods catalysts were uncovered. The photothermal catalytic activity of CuCeO 2−x nanorods doped with 10 wt% Cu reaches to 90% CO conversion under Xe lamp illumination (2.5 suns), and the solar driven photothermal CO-PROX reaction on CuCeO 2−x nanorods were proposed to be proceeded by the light-to-thermal conversion and subsequently to drive a thermal catalytic process. The catalytic performance of CuCeO 2−x nanorods in photothermal CO-PROX is closely related to the photo-to-thermal conversion efficiency and Cu-Ce synergetic interaction of CuCeO 2−x nanorods catalyst. The introduction of CuO x greatly broaden the optical absorption range and promotes the light absorption capacity of ceria nanorods, which induces the catalyst with high photo-to-thermal conversion capability. Moreover, the optimal copper dopant benefits to enhance the Cu-Ce synergetic interaction and accelerate the oxidation reaction taking place at low temperature. CuCeO 2−x nanorods catalyst shows promising competitive activity and ultra-low cost compared with the noble-based catalyst for the purification of hydrogen streams by the clean and eco-friendly sunlight sources.
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Catalysts
·
2024
·Vol. 14
·期 3
·183
·
IF 3.8
Jiarong Ma,Run Zhou,Yu Tu,Ruixin Ma,Daimei Chen,Hao Ding
Ni3Si2O5(OH)4rods (NS) were synthesized via a hydrothermal method, employing natural wollastonite as a template. The hierarchical Ni3Si2O5(OH)4rods exhibited vertically oriented nanosheets, resulting in a substantial increase in the specific surface area (from 2.24 m2/g to 178.4 m2/g). Subsequently, a CdS/Ni3Si2O5(OH)4composite photocatalyst (CdS/NS) was prepared using a chemical deposition method. CdS was uniformly loaded onto the surface of the Ni3Si2O5(OH)4nanosheets, successfully forming a heterojunction with Ni3Si2O5(OH)4. The CdS/NS photocatalyst in the presence of lactic acid as a sacrificial agent demonstrated an impressive H2production rate of 4.05 mmol h−1g−1, around 40 times higher than pure CdS. The photocorrosion of CdS was effectively solved after loading. After four cycles, the performance of CdS/NS remained stable, showing the potential for sustainable applications. After photoexcitation, electrons moved from Ni3Si2O5(OH)4to the valence band of CdS, where they interacted with the holes via an enhanced interface contact. Simultaneously, electrons in CdS transitioned to its conduction band, facilitating hydrogenation. The enhanced performance was attributed to the improved CdS dispersion by Ni3Si2O5(OH)4loading and efficient photogenerated carrier separation through the heterojunction formation. This work provides new perspectives for broadening the applications of mineral materials and developing heterojunction photocatalysts with good dispersibility and recyclability.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2025
·
IF 14.3
Mian Wei,Xin Zhou,Chang Cheng,Jianjun Zhang,Chuanjia Jiang,Bei Cheng
Graphitic carbon nitride is flourishing in photocatalytic hydrogen production. However, the performance of traditional carbon nitride materials is limited by their scarcity of surface reactive sites and fast recombination of photogenerated electron-hole pairs. Herein, we introduce a simple ultrasonic synthesis method that exfoliates bulk carbon nitride into nanosheets while simultaneously forming S-scheme heterojunctions with in-situ grown thiophene-based polymer through π–π interactions. The obtained carbon nitride nanosheet/polymer S-scheme heterojunction possesses abundant surface active sites and exhibits suppressed recombination of photogenerated electron-hole pairs, resulting in a hydrogen production rate approximately double that of bulk carbon nitride and a superior apparent quantum yield of 5.00%. The S-scheme charge transfer mechanism was proven by in-situ irradiated X-ray photoelectron spectroscopy, and time-resolved femtosecond-transient absorption analysis clarified the charge separation and transfer dynamics. This study demonstrates that combining organic semiconductors and hypercrosslinked polymers is a promising strategy for designing highly efficient S-scheme heterojunction photocatalysts.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Jiawen Wang,Jinfu Wang,Zi Wang,Jiayue Wu,Jiaxuan Liao,Shenyuan Zhan,Xiaoye Chen,Xinhao Wang,Yongbao Wei,Qidong Zhou,Liefu Ye,Jinfeng Wu
Incontinence-associated dermatitis (IAD) leads to persistent tissue damage, antibiotic-resistant infections, and neurogenic inflammation, greatly impairing patients' quality of life. Current therapies fail to simultaneously eliminate resistant bacterial biofilms, neutralize alkaline conditions, and break the cycle of ammonia (NH 3 ) regeneration. Here, a piezoelectric gas therapy strategy based on platinum-decorated bismuth molybdate load in gelatin methacrylate (GelMA) hydrogel (Pt@BMO-Gel) is introduced. Under ultrasound excitation, Pt@BMO generates high piezoelectric potential to improve charge separation, selectively adsorbs NH 3 on BMO (001) crystal facets, efficiently degrades NH 3 to normalize pH, and enables sustained release of H 2 and NO for dual antibacterial and anti-inflammatory effects. Mechanistic insights from theoretical calculations show that the Pt (111) and BMO (001) surfaces lower energy barriers for H 2 formation and N─H bond cleavage, conducive to the generation of NO and H 2 . Transcriptomic profiling reveals downregulation of key nitrogen metabolism genes (arcC/hutH) in methicillin-resistant Staphylococcus aureus (MRSA) and disruption of the (p)ppGpp-mediated stringent response, effectively eradicating bacterial persistence via metabolic reprogramming. This study establishes Pt@BMO as an efficient piezoelectric catalyst for wound therapy, presenting a novel approach in medicine that transforms harmful NH 3 into therapeutic H 2 and NO, offering a promising treatment paradigm for infected wounds, such as incontinence-associated dermatitis.
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高影响因子
FUEL
·
2025
·
IF 7.5
Ying Li,Haibo Zhao
Ethylene production via chemical looping oxidative dehydrogenation (CL-ODH) of ethane faces a critical challenge in balancing conversion efficiency and selectivity due to competing oxygen species requirements. Here, we present a bifunctional composite catalyst (CrH/BiCZ) by physically integrating a Cr-HZSM5 (Cr-H) dehydrogenation (DH) catalyst with a Bi 2 O 3 -Ce 0.4 Zr 0.6 O 2 (Bi-CZ) selective hydrogen combustion (SHC) catalyst. This tandem system decouples ethane activation and hydrogen combustion, promoting the DH process of ethane through the in situ hydrogen combustion of the SHC catalyst. The Ce-Zr solid solution in Bi-CZ acts as an oxygen reservoir, enabling complete H 2 combustion within 3 min and suppressing carbon deposition. This rapid hydrogen combustion shifts the reaction equilibrium towards ethylene production. At 650 °C, the optimized CrH/BiCZ catalyst achieves 84.1 % ethylene selectivity at 43.0 % ethane conversion, and maintains exceptional stability over 36 redox cycles. This work establishes a scalable chemical looping strategy for efficient ethylene synthesis.
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高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Guoxin Jiang,Shenghui Guo,Guangyu Chen,Hao Sun,Runan Jia,Ming Hou,Li Yang
Hydrogen becomes an important clean energy origin, which will explode in open fire at a certain concentration. This leads to great property and personal safety hazards in the process of hydrogen storage, transportation and leakage. Low temperature and low concentration hydrogen detection is very necessary. In this paper, MXene-TiO 2 -ZnO ternary composites were successfully prepared by one-step in-situ oxidation method using MXene and Zn(NO 3 ) 2 ·6H 2 O as precursors for 1h. The microstructure of the samples was characterized by XPS, TEM, SEM and Raman, and their gas sensing properties were tested. The results show that the Ti 3 C 2 T x -TiO 2 -ZnO structure exhibits a layered accordion-like morphology. Under room temperature (RT 25 °C) and UV light irradiation, the response value of MTZ-1 sample to 1000 ppm hydrogen reaches 73.39 %, which is 96.8 % higher than that of pure Ti 3 C 2 T X . At the optimum operating temperature (100 °C), the response value of MTZ-1 to 1000 ppm hydrogen reached 96.77 %, the detection limit was as low as 1 ppm, and the response value was 1.7 %. The results show that the formation of TiO 2 -ZnO heterojunction, the retention of Ti 3 C 2 T x layered structure and UV irradiation are the main reasons to improve the gas sensing performance (GSP). In this paper, the formation of TiO 2 -ZnO heterojunction, the retention of MXene layered structure and the synergistic enhancement of gas sensitivity by UV excitation were revealed by systematic characterization and mechanism analysis. This research provides a new idea for the development of low energy consumption and high sensitivity room temperature hydrogen sensor, which has important practical application value.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Hang Xu,Ningxiang Lan,Yan Hu,Yuchun Xi,Jinzhi Hu,Chaowei Wen,Wanpeng Li,Chuanqiang Yin,Xiaomin Li,Lang Zhou
In this study, a novel polyimide (PI)/metal-organic frameworks (MOFs)/polyetherimide (PEI) composite membrane was fabricated for gas separation applications. The directional alignment of MOFs on PI electrospun nanofibers was achieved by an in-situ growth method, resulting in the construction of continuous, fast, and low-resistance gas transport channels in the composite membrane (PEI/PI@ZIF-67). This PI nanofiber backbone with a three-dimensional network structure not only remarkably enhanced the interfacial compatibility between the polymer and the MOFs, but also significantly improved the mechanical strength of the membrane, resulting in a tensile strength of the composite membrane of 100 MPa. Moreover, the introduction of PI fibers promoted the oriented alignment of the MOFs and enhanced the H 2 separation performance. The H 2 permeability of PEI/PI@ZIF-67-3 was 9.5 Barrer, which was 439% higher than that of the pure PEI membrane. The H 2 /CO 2 selectivity was 9.3, which was 3.3 times higher than that of the pure PEI membrane. This can be attributed to the porous structure of ZIF-67 and the complex and tortuous gas transport path provided by the PI fibers, allowing the optimized composite design of PEI/PI@ZIF-67 to simultaneously improve gas permeability and selectivity. Furthermore, the prepared fiber composite membranes exhibited good hydrophobicity and thermal stability. Consequently, PEI/PI@ZIF-67, with its continuous and fast transport path, shows great potential for CO 2 capture and H 2 recovery applications.
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