Nanomaterials
·
2020
·Vol. 10
·期 12
·2449
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IF 4.324
Shiliang Heng,Lei Li,Weiwei Li,Haiyan Li,Jingyu Pang,Mengzhen Zhang,Yan Bai,Dongbin Dang
The development of high-efficiency, recyclable, and inexpensive photocatalysts for water splitting for hydrogen production is of great significance to the application of solar energy. Herein, a series of graphene-decorated polyoxoniobate photocatalysts Nb6/PPy-RGO (Nb6= K7HNb6O19, RGO = reduced graphene oxide, PPy = polypyrrole), with the bridging effect of polypyrrole were prepared through a simple one-step solvothermal method, which is the first example of polyoxoniobate-graphene-based nanocomposites. The as-fabricated photocatalyst showed a photocatalytic H2evolution activity without any co-catalyst. The rate of 1038 µmol g−1in 5 h under optimal condition is almost 43 times higher than that of pure K7HNb6O19·13H2O. The influencing factors for photocatalysts in photocatalytic hydrogen production under simulated sunlight were studied in detail and the feasible mechanism is presented in this paper. These results demonstrate that Nb6O19acts as the main catalyst and electron donor, RGO provides active sites, and PPy acted as an electronic bridge to extend the lifetime of photo-generated carriers, which are crucial factors for photocatalytic H2production.Keywords:polyoxoniobate;Nb6/PPy-RGO composites;electronic bridge;H2production
研究领域:
材料科学
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能源科学
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产品关联
DOI
PubMed
高影响因子
MATERIALS RESEARCH BULLETIN
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2023
·
IF 5.4
Tao Wang,Jinyu Wang,Chunlan Li,Yu Wu,Yuxuan Sun,Xiqing Liu,Xiaoli Su,Hongquan Zhan,Yongqing Wang
Carbon materials can act as electron transfer media to effectively enhance photocatalytic performance. In this study, carbon dots (CDs) were prepared using green tea to modify Ni 2 P/NiCo-LDH heterostructures. Benefitting from the Co-P bond formed between Ni 2 P and NiCo-LDH and biomass CDs, charge transfer was improved via dual channel. Ni 2 P and CDs acted as active sites for improving the photocatalytic performance. Owing to the synergistic process, the photoresponse capability of CDs/Ni 2 P/NiCo-LDH was significantly increased. In addition, the possible active species in the photocatalytic process are discussed. This study provides a design for ternary photocatalysts with carbon materials and phosphides.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Yubo Wu,Honglin Lin,Xuyun Gao,Zhiyan Liu,Yulun Nie
The Fe 3+ /Fe 2+ cycle has been identified as the rate-limiting step in the Fenton system, and many efforts have been made to promote the Fe 3+ reduction via external electrons provided by various electron donors. However, how to design an efficient electron transport pathway and then inhibit the invalid electron shuttle has been largely underestimated. In this study, two kinds of heterogeneous Fenton catalysts of CuO@Fe 2 O 3 and CuO@C@Fe 2 O 3 were prepared. The key role of carbon in transporting electrons as an electron bridge and its enhancement mechanism in photo-assisted Fenton-like performances were explored in detail. Compared with CuO@Fe 2 O 3 , the removal efficiency of tetracycline (TC) and the corresponding pseudo-first order reaction rate constants over CuO@C@Fe 2 O 3 increased significantly from 88.6 % and 0.1054 min −1 to 99.7 % and 0.2058 min −1 , respectively. Based on a series of probe experiments, visible light irradiation can promote the reduction of Cu 2+ to Cu + , then the carbon in CuO@C@Fe 2 O 3 can effectively transfer electrons from Cu + to Fe 3+ , enhancing the Fe 3+ /Fe 2+ cycle and the following Fenton-like efficiency. Since more ·OH while less ∙O 2 - was produced over CuO@C@Fe 2 O 3 , which further supports the fact that the enhanced Fe 3+ /Fe 2+ cycle was due to the transfer electron from Cu + to Fe 3+ instead of the Haber-Wiss mechanism. Hence, this study provides new insight for effectively improving the transfer efficiency and effective utilization of electrons in Fenton systems.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Xiaolong Wu,Mingnv Guo,Ziqi Wang,Ruiming Fang,Jiang He,Zhongqing Yang
For the purpose of further improve the efficiency of photocatalytic CO 2 reduction and realize cascade utilization of the full solar spectrum, Bi 2 MoO 6 quantum dots were in situ deposited on the surface of carbonized pomelo peel (CPP) to form Bi 2 MoO 6 @CPP 0D/3D heterojunction catalyst. With a diameter of less than 10 nm, the quantum-limited field effects confirm the successful construction of Bi 2 MoO 6 quantum dot. The band structure of Bi 2 MoO 6 @CPP 0D/3D is beneficial heterojunction , which is able to utilize not only the UV–Vis band to generate photogenerated carriers that reduce CO 2 to CO mainly, but also the IR band of the solar spectrum to increase the temperature of photothermal catalytic reaction. The experiment indicated that the photogenerated electrons generated by Bi 2 MoO 6 @CPP 0D/3D heterojunction catalysts flowed through the interface C-O-Bi bridge and migrated to the surface of CPP, forming an electron interface. The interface C-O-Bi electron bridge enhanced the separation ability of photogenerated carriers, thereby increasing the CO yield to 50.77 μmol/(g·h). Further experiment showed that the oxygen-containing groups’ concentration of CPP were ameliorated by thermal activation and acid-base activation, which increased the concentration of interface C-O-Bi electron bridge between Bi 2 MoO 6 and CPP, finally promoting the CO yield to 66.94 μmol/(g·h), which is 12.3 times greater than that of bulk Bi 2 MoO 6 .
研究领域:
材料科学
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环境科学
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光催化
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DOI
高影响因子
ACS Applied Energy Materials
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2023
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IF 6.4
Mingnv Guo,Ziqi Wang,Xiaolong Wu,Jiaqi Qiu,Linlin Gu,Zhongqing Yang
The carrier migration limitation has been a key factor restricting the photothermal catalytic CO2 reduction. To further enhance carrier transport, Bi2MoO6 quantum dots (BM QDs) are deposited on the surface of alkali-activated pomelo-peel-derived carbon (CPP-A) to construct CPP-A/BM QDs 0D/3D heterojunctions in this paper. BM QDs have extremely short carrier transport distances and achieve photothermal synergy through the graded utilization of the full solar spectrum. The carbon framework of CPP promotes the high dispersion of BM QDs (3 nm) and allows the local surface temperature of the catalyst to increase rapidly up to 100 °C. The critical role of heat enhances the diffusion, adsorption, and carrier migration processes of CO2 and provides the energy to cross the CO2 activation energy barrier. More importantly, the oxygen-containing groups of CPP and BM QDs form a C–O–Bi interfacial electron bridge, which provides a high-speed channel for carrier transport across the interface, allowing many electrons generated by BM QDs to migrate rapidly to the CPP surface, inducing CPP as a new electron-rich surface for rapid CO2 activation, which results in an ultrahigh CO yield of 61.44 μmol/(g·h) for CPP-A/BM QDs, and the catalytic activity is increased by 9.12 times.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Shaosheng Rao,Yangyang Sun,Juan Xie,Chenglong Chen,Chuang Zhi,Rong Ma,Qinqin Liu,Juan Yang
Although photocatalytic disinfection can avoid secondary pollution and other shortcomings compared to traditional disinfection methods, its development is seriously hindered by poor charge separation and transfer efficiency. Herein, we design a Zn-NC (single Zn atoms embedded in nitrogen-doped carbon) bridged ZnO/C 3 N 4 Z-scheme heterojunction (ZnO/Zn-NC/C 3 N 4 ) with robust interface contact by a multi-interfacial engineering strategy to achieve highly efficient separation and transfer of charge. Experimental and theoretical analyses demonstrate that the tightly integrated interface and excellent electrical conductivity of Zn-NC electron bridges ensure effective transfer of photogenerated charge carriers. Compared to ZnO/C 3 N 4 , the introduction of Zn-NC electron bridges induces charge rearrangement at the interface, generating a strong built-in electric field in the ZnO/Zn-NC/C 3 N 4 Z-scheme heterojunction to facilitate the separation and transfer of photogenerated charge carriers. Furthermore, Zn-NC electron bridges effectively promote the adsorption and activation of oxygen on the surface of ZnO/Zn-NC/C 3 N 4 , enhancing the generation of reactive oxygen species for rapid bacteria elimination in water. Consequently, the ZnO/Zn-NC/C 3 N 4 Z-scheme heterojunction, at a concentration of 100 ppm, achieves 99.9 % antibacterial efficiency against methicillin-resistant Staphylococcus aureus , Staphylococcus aureus , and Escherichia coli at a bacterial concentration of ∼ 10 7 CFU/mL under AM 1.5G simulated sunlight irradiation for 60 min, which is approximately 1.05 times higher than that of ZnO/C 3 N 4 . Moreover, ZnO/Zn-NC/C 3 N 4 maintains a 99.9 % bactericidal efficiency for natural water treatment using a homemade microreactor, demonstrating its potential for water disinfection.
研究领域:
环境科学
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材料科学
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微生物学
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DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2025
·Vol. 54
·期 48
·17998-18008
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IF 3.3
Jianding Li,Jinwen Wu,Min Li,Yanling Hu,Yifeng Du,Xueqing Yu,Huajun Zhao,Yinan Huang,Liqing He
To further enhance the electrocatalytic performances of Pd-based electrocatalysts in small organic molecule oxidation reactions, Pd/C was modified by a redox-active organic molecule (9,10-phenanthrenequinone, PQ), resulting in a novel Pd/C-PQ catalyst. The catalyst was prepared by first physically adsorbing PQ onto the surface of Vulcan XC-72 carbon black (C-PQ), followed by the deposition of Pd nanoparticles on this modified C-PQ support. Results demonstrated that the Pd nanoparticles within the Pd/C-PQ catalyst were well-dispersed with a particle size distribution ranging from 2.4 to 4.6 nm. This size was significantly smaller than that of Pd nanoparticles in the unmodified Pd/C catalyst. Electrochemical testing revealed a substantial enhancement in performance. The mass and specific activity for formic acid oxidation achieved by the Pd/C-PQ catalyst were 2.67 and 2.07 times higher than that of the unmodified Pd/C catalyst, respectively. In addition, the CO stripping peak of the Pd/C-PQ catalyst exhibited a negative shift of 26 mV compared to Pd/C, indicating weaker CO adsorption. The remarkably improved stability was also observed for the Pd/C-PQ catalyst. Furthermore, the charge transfer kinetics for the formic acid oxidation reaction were significantly accelerated. The enhanced electrochemical performance of the Pd/C-PQ catalyst can be attributed to several synergistic factors of uniformly dispersed Pd with relatively smaller particle sizes, electronic interaction/modification between Pd and PQ, and the cooperative role of the PQ molecules acting as efficient redox mediators.
研究领域:
电化学
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催化化学
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纳米材料
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能源化学
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表面科学
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产品关联
DOI
PubMed
高影响因子
DESALINATION
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2023
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IF 9.9
Xueying Gao,Zhenzhen Fu,Yanfei Sun,Dewei Wang,Xiaoxuan Wang,Zishan Hou,Jinrui Wang,Xia Liu,Shiyu Wang,Shuyun Yao,Huiying Zhang,Shuyuan Li,Zheng Tang,Weijie Fu,Kaiqi Nie,Jiangzhou Xie,Zhiyu Yang,Yi-Ming Yan
While MnO 2 has been identified as a potent agent in the desalination process , its efficacy is significantly impeded by its inherent poor electrical conductivity and substantial ion diffusion barriers . By orchestrating an interfacial electron bridge within the MnO 2 /g-C 3 N 4 heterostructure , reinforced through N p z -Mn d z 2 orbital hybridization, we have managed to significantly boost both SAC and SAR in the HCDI process. The reinforced N p z -Mn d z 2 orbital hybridization triggers a substantial electron transition from g-C 3 N 4 to MnO 2 , culminating in a high Mn d z 2 electron occupancy. Further analysis reveals the formation of a Mn N chemical bond at the MnO 2 /g-C 3 N 4 interface, operating as an essential electron transfer bridge from g-C 3 N 4 to MnO 2 . This process concurrently initiates a rise in the Mn d z 2 orbital energy level, equipping the Mn d z 2 electron with superior redox activity. With these enhancements, the manufactured MnO 2 /g-C 3 N 4 exhibits exemplary performance, boasting an improved SAC of 68 mg g −1 and SAR of 3.6 mg g −1 min −1 with a decreased energy consumption of 0.7224 kWh kg −1 at 1.2 V. This innovative work offers an unconventional roadmap for activating electron redox activity and thereby accelerating charge transfer in transition metal oxides .
研究领域:
材料科学
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环境科学
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电化学
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水处理
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Wenxin Wang,Ruidong Yang,Qiqi Mao,Xu Mu,Hongjie Yu,Kai Deng,Jianguo Wang,Liang Wang,Hongjing Wang
The utilization of green hydrogen sources in H 2 O for alkynols electrocatalytic semihydrogenation reaction (ESHR) at ambient temperature provides a promising pathway toward the sustainable conversion of alkynols. However, it is still a great challenge to construct specific interfacial structure to adjust the electronic structure of Pd for the purpose of altering the strong adsorption of Pd with active hydrogen to enhance the production of alkenols. Here, the atomically dispersed GaO x -PdMo bimetallene nanoribbons (GaO x -PdMo BNRs) via oxygen bridging Ga atoms is designed to the surface of PdMo BNRs for 2-methyl-3-butyn-2-ol (MBY) ESHR to the synthesis of 2-methyl-3-buten-2-ol (MBE). The GaO x -PdMo BNRs achieve the excellent MBE selectivity (≈97.4%), Faraday efficiency (≈96.1%), and maintain long-term stability. Density functional theory demonstrates that the top electron-enriched Ga atoms and the bottom electron-deficient Pd atoms construct a “pyramidal” interface via the oxygen bridge. The unique surface can effectively activate H 2 O and weaken interaction between catalyst and MBE, thus promoting MBE generation. Moreover, the electron bridge effect between Ga-O-PdMo can induce p-d orbital hybridization to achieve lower the d -band center of surface Pd thus modulating the reactants adsorption. This work provides a strategy to improve ESHR performance by electron bridge effect to modulate interfacial electron distribution.
研究领域:
材料科学
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催化化学
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理论计算
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产品关联
DOI
高影响因子
Small
·
2023
·Vol. 19
·期 39
·2302330
·
IF 13.3
Rui Du,Chuantao Wang,Li Guo,Razium Ali Soomro,Bin Xu,Chunming Yang,Feng Fu,Danjun Wang
Selective oxidation of biomass-based molecules to high-value chemicals in conjunction with hydrogen evolution reaction (HER) is an innovative photocatalysis strategy. The key challenge is to design bifunctional photocatalysts with suitable band structures, which can achieve highly efficient generation of high-value chemicals and hydrogen. Herein, NiS/Cd 0.6 Zn 0.4 S Schottky junction bifunctional catalysts are constructed for sunlight-driven catalytic vanillyl alcohol (VAL) selective oxidation towards vanillin (VN) coupling HER. At optimal conditions, the 8% NiS/Cd 0.6 Zn 0.4 S photocatalyst achieves high activity of VN production (3.75 mmol g −1 h −1 ) and HER (3.84 mmol g −1 h −1 ). It also exhibits remarkable VAL conversion (66.9%), VN yield (52.1%), and selectivity (77.8%). The photocatalytic oxidation of VAL proceeds a carbon-centered radical mechanism via the cleavage of α C–H bond. Experimental results and theoretical calculations show that NiS with metallic properties enhances the electron transfer capability. Importantly, a Ni-S-Cd “electron bridge” formed at the interface of NiS/Cd 0.6 Zn 0.4 S further improves the separation/transfer of electrone/h + pairs and also furnishes HER active sites due to its smaller the |ΔG H* | value, thereby resulting in a remarkably HER activity. This work sheds new light on the selective catalytic oxidation VAL to VN coupling HER, with a new pathway towards achieving its efficient HER efficiency.
研究领域:
材料科学
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催化化学
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太阳能利用
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产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yongqi Chen,Xiaochun Wang,Jingen Zhou,Sifan Shao,Song Wang,Qingshu Wang,Zhonghua Wang,Dong Li,Haiqian Zhao
Conventional carbon-based sorbents, such as activated carbon, exhibit limited formaldehyde uptake due to a lack of sufficient specific binding sites. In contrast, calcium single-atom adsorbents anchored on porous carbon significantly enhance formaldehyde capture; however, the role of the coordination environment in this process remains insufficiently understood. Here, we report a coordination-environment-regulated carbon-supported calcium single-atom adsorbent that markedly improves formaldehyde adsorption. The adsorption behavior of calcium single-atom adsorbents was systematically investigated through a combination of density functional theory (DFT) calculations and static adsorption experiments. A clear linear correlation was identified between the number of oxygen ligands in the divacancy configuration and the adsorption energy. Among the studied configurations, the tetra-oxygen-coordinated Ca/DV-O 4 structure exhibited the highest adsorption energy (-1.90 eV), demonstrating superior performance. Comprehensive geometric optimization, charge-density difference, and density-of-states analyses revealed that the enhanced adsorption arises from the electron-bridging role of calcium and the strengthened hybridization between Ca-3d and O-2p orbitals. In static adsorption experiments, the Ca/DV-O 4 configuration achieved an equilibrium removal efficiency of 63.5 %, representing a 51.2 % improvement compared to conventional activated carbon. This work elucidates the adsorption mechanism of calcium single-atom adsorbents toward formaldehyde and provides design principles for the rational manipulation and optimization of calcium single-atom coordination environments.
研究领域:
环境化学
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材料科学
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物理化学
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吸附科学
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计算化学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Dong Yan,Xuetao Cheng,Xiaoxiao Dong,Han Wang,Xingchen Chang,Chenghui Xia,Yongcheng Jin,Chun-Chao Hou
Electrolysis of seawater driven by renewable energy holds great promise for sustainable hydrogen production. However, both catalyst corrosion caused by competitive Cl − adsorption and sluggish reaction kinetics are major challenges in seawater electrolysis. Here, inspired by the concept of hard and soft acids and bases (HSAB), a unique interfacial W-O-Co electron bridge is constructed on the catalyst surface to achieve the electronic coupling of hard-acid W site and borderline-acid Co site via the oxygen bridge, which demonstrates exceptional performance for both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) in alkaline water and seawater, as well as high anti-corrosion stability. Remarkably, WO 3 /CoP electrode requires low overpotentials of merely 154 mV (alkaline freshwater) and 189 mV (alkaline seawater) for HER, and 334 mV (alkaline freshwater) and 343 mV (alkaline seawater) for OER to achieve 100 mA cm −2 , respectively. When deployed our bifunctional catalyst as both anode and cathode in an alkaline anion-exchange membrane seawater electrolyzer, the system achieves 1 A cm −2 at a low cell voltage of 1.80 V and maintains stable electrolysis for over 250 h at 100 mA cm −2 . Theoretical and experimental investigations reveal that the hard-acid W site of the electronic W-O-Co bonded bridge prefers adsorption of hard-base OH - rather than soft-base Cl - , thereby mitigating Cl - interference and suppressing chloride corrosion. Simultaneously such interfacial W-O-Co bridging significantly accelerates charge transfer from Co site to W site, thereby regulating the electronic structures of catalysts and optimizing the sorption behaviors of reaction intermediates. This work provides a feasible anti-corrosion engineering strategy to design efficient and robust electrocatalysts for practical seawater electrolysis.
研究领域:
电化学
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材料科学
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氢能
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催化
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可再生能源
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）