Catalysis Science & Technology
·
2023
·Vol. 13
·期 7
·2101-2107
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IF 5
Jianhao Qiu,Lu Zhang,Guanglu Xia,Dingliang Dai,Yong Tang,Jianfeng Yao
Different ligand functionalized UiO-66 (UiO-66-X, X = OH, (OH)2 and NH2) were prepared and then modified by ZnIn2S4 lamellas to form ZnIn2S4/UiO-66-X heterostructures for visible-light-driven H2O2 evolution in pure water. The H2O2 yields using ZnIn2S4/UiO-66-NH2, ZnIn2S4/UiO-66-(OH)2 and ZnIn2S4/UiO-66-OH are 799, 733 and 165 μmol L−1, respectively, which are 9.5, 8.7 and 2.0 times that of ZnIn2S4/UiO-66. The high performance of ZnIn2S4/UiO-66-NH2 and ZnIn2S4/UiO-66-(OH)2 is ascribed to the benign visible-light response and Z-scheme heterostructures, and the H2O2 evolution abides by indirect O2 reduction with ˙O2− as an intermediate species. Additionally, H2O2 yields using ZnIn2S4/UiO-66-NH2 on tap water and Xuanwu Lake (Nanjing, China) water can be comparable to that on the above-deionized water. This study sheds light on the great promise of functionalized MOFs and their applications on green (photo)catalytic energy conversion.
研究领域:
材料科学
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光化学
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环境科学
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产品关联
DOI
高影响因子
CARBON
·
2022
·
IF 11.307
Yuanyuan Shao,Jundie Hu,Tingyu Yang,Xiaogang Yang,Jiafu Qu,Qi Xu,Chang Ming Li
Hydrogen peroxide (H 2 O 2 ) is an important green oxidant for environmental remediation. It is a sustainable strategy to realize solar-driven in- situ H 2 O 2 production for timely using via cascade reactions to sterilization or remove organic pollutants etc. However, how to improve the H 2 O 2 production and consumption abilities of catalysts are the two main challenges. Here we report a superior carbon-related ZnIn 2 S 4 /g-C 3 N 4 catalyst with excellent H 2 O 2 generation and consumption capabilities for efficient sterilization under visible light irradiation. The 2D/2D heterojunction of ZnIn 2 S 4 /g-C 3 N 4 with rapid carrier separation and transfer efficiency exhibits a remarkable H 2 O 2 yield of 4.27 mmol g −1 , which is much higher than that of current catalysts. The in- situ produced H 2 O 2 can be quickly activated to strong oxidizing hydroxyl radicals for sterilization, in which the Escherichia coli ( E. coli ) are fully cleared only within 25 min and 98% of Staphylococcus aureus ( S. aureus ) are killed out after 60 min irradiation. The prepared photocatalysts realize the rapid production and consumption of H 2 O 2 , and this work provides an effect green strategy for sterilization via the in- situ generated H 2 O 2 .
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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生物技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 43
·22720-22727
·
IF 11.301
Xueming Dang,Ruying Yang,Zhe Wang,Siyi Wu,Huimin Zhao
Graphitic carbon nitride (g-C3N4) possesses unique electronic and optical properties in the visible-light-driven production of H2O2. However, bulk g-C3N4 suffers from inefficient sunlight absorption and low carrier mobility. Herein, P doped g-C3N4 with a hollow sphere architecture was synthesized. The hollow sphere structure provides a large accessible surface area for charge transfer and enhances photo-absorption properties. Particularly, the doped P can regulate the energy band structure with stronger reducibility for O2 activation and accelerate photo-generated carrier separation. Meanwhile, the P heteroatom is beneficial to produce 1,4-endoperoxide species more easily and enhance selectivity for H2O2 synthesis through a two-electron O2 reduction process. The resultant catalyst exhibits a high H2O2 production rate of 174 μmol h−1 g−1 in pure water and 1684 μmol h−1 g−1 with isopropanol as a hole scavenger, which are 7.5 and 11.2 times those of bulk g-C3N4. This work provides a new avenue for the design and modification of other photocatalysts for H2O2 production.
研究领域:
材料科学
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光化学
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催化
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Yong Tang,Jianhao Qiu,Dingliang Dai,Guanglu Xia,Yixin Li,Biyao Fang,Jianfeng Yao
Sluggish charge transfer dynamics are still the key issue limiting the development of photocatalysis. In this study, CdS/ZnIn 2 S 4 /MIL-53-NH 2 ternary hierarchical heterostructures were constructed via a building block approach, where ZnIn 2 S 4 lamellae first grow on MIL-53-NH 2 followed by CdS nanoparticle deposition. The favorable interfacial compatibility and ternary heterostructures contribute to rapid and multistep spatial charge transfer, which suppresses charge recombination. Therefore, ultrahigh H 2 O 2 production of 1792 μmol·L −1 was obtained over CdS/Znln 2 S 4 /MIL-53-NH 2 composites with visible light, pure water and ambient air, which is not only higher than that of each monomer and binary heterostructure but also better than those of most reported references. Notably, the apparent quantum yield reached 4.5 % at 400 nm, and the solar-to-H 2 O 2 conversion efficiency was 0.081 % in pure water and ambient air. Additionally, H 2 O 2 generation over CdS/Znln 2 S 4 /MIL-53-NH 2 composites involves two-electron O 2 reduction with ·O 2 - as an intermediate. This work may encourage heterostructure design for efficient photocatalytic H 2 O 2 production.
研究领域:
材料科学
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光催化
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纳米技术
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化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2022
·Vol. 119
·期 32
·e2209056119
·
IF 12.779
Bolei Chen,Yu Xia,Rongxiang He,Hongqian Sang,Wenchang Zhang,Juan Li,Lufeng Chen,Pu Wang,Shishang Guo,Yongguang Yin,Ligang Hu,Maoyong Song,Yong Liang,Yawei Wang,Guibin Jiang,Richard N. Zare
Contact electrification between water and a solid surface is crucial for physicochemical processes at water–solid interfaces. However, the nature of the involved processes remains poorly understood, especially in the initial stage of the interface formation. Here we report that H2O2 is spontaneously produced from the hydroxyl groups on the solid surface when contact occurred. The density of hydroxyl groups affects the H2O2 yield. The participation of hydroxyl groups in H2O2 generation is confirmed by mass spectrometric detection of 18O in the product of the reaction between 4-carboxyphenylboronic acid and 18O–labeled H2O2 resulting from 18O2 plasma treatment of the surface. We propose a model for H2O2 generation based on recombination of the hydroxyl radicals produced from the surface hydroxyl groups in the water–solid contact process. Our observations show that the spontaneous generation of H2O2 is universal on the surfaces of soil and atmospheric fine particles in a humid environment.
研究领域:
物理化学
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环境科学
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表面科学
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产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2024
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IF 11.3
Jiayu An,Wenjun Jiang,Fuwei Zhuang,Yinhua Ma,Su Zhan,Feng Zhou
Utilizing photocatalytic technology to achieve efficient production of H2O2 is a hot topic. Here, we synthesized a photocatalytic material with a strong built-in electric field, namely, Pym-CN, through a hydrothermal-assisted thermal polymerization strategy, which effectively promotes the separation and transfer of photoinduced charge carriers. A pyrimidine ring was successfully introduced into the heptazine structure unit of Pym-CN, which leads to electron aggregation at N═C–N, benefiting for enhancing the strong sorption and activation capabilities of oxygen. Under the condition of visible light wavelength greater than 400 nm (λ > 400 nm), the H2O2 production rate of Pym-CN (2622.5 μmol/L/h) is 7.6 times that of the BCN. A detailed investigation of the reaction mechanism revealed that Pym-CN follows a two-step continuous process of single-electron oxygen reduction reaction (ORR). This work elucidates the application prospects of the donor–acceptor (D–A) structure with a strong built-in electric field in the field of efficient photocatalytic production of H2O2.
研究领域:
材料科学
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光催化
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可再生能源
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化学工程
✓ 已验证
DOI
高影响因子
ACS Nano
·
2024
·
IF 15.8
Xu Li,Wenlong Tan,Jinsong Fan,Kun Li
Although the past decade has witnessed a rapid development of oxidoreductase-mimicking nanozymes, the mimicry of cofactors that play key roles in mediating electron and proton transfer remains limited. This study explores how surface Au–H species conjugated to Au nanoparticles (NPs) that imitate formate dehydrogenase (FDH) can serve as cofactors, analogous to NADH in natural enzymes, offering diverse possibilities for FDH-mimicking Au nanozymes to mimic various enzymes. Once O2 is present, Au–H species assist Au NPs to complete the on-demand H2O2 generation for cascade reactions. Alternatively, when oxidizing organic molecules are introduced as substrates, Au–H species confer nitro reductase- and aldehyde reductase-like activities on Au NPs under anaerobic conditions. Furthermore, similar to the dehydrogenase–NADH complex, Au NPs possessing Au–H species are gifted with esterase-like activity for ester hydrolysis. By revealing that Au–H species are prosthetic groups for FDH-mimicking Au nanozymes, this work may inspire explorations into future self-generated cofactor mimics for nanozymes, thereby circumventing the need for exogenous cofactors.
研究领域:
催化
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生物化学
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纳米技术
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酶学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Jianguo Wu,Haoxiang Xu,Dong Cao,Daojian Cheng
Supported PdAu bimetallic nanoparticles have been developed for the direct synthesis of H 2 O 2 (DSHP). However, to date, the dilute H 2 streams necessary to avoid potential risks of explosion limits the attainable product concentrations of H 2 O 2 . Here, a series of silicon-modified Al 2 O 3 (Si x Al) were synthesized for loading PdAu bimetallic nanoparticles . The H 2 consumption turnover frequency (TOF) and H 2 O 2 formation TOF show a volcano trend with the silica content, where PdAu/Si 5.6 Al exhibits the best H 2 consumption TOF and H 2 O 2 formation TOF (11259.3 and 1995.2 h −1 ). Silica on the surface of Al 2 O 3 is identified as Brønsted (B) acid site. The increase of B acid sites density accelerates the H 2 conversion into H atoms, thereby boosting H 2 O 2 formation process. The adsorption and dissociation of H 2 into atomic H at B acid sites would spill across the support to PdAu nanoparticles reversely. The reversed hydrogen spillover effect induced by B acid site accounts for enhanced H 2 conversion and H 2 O 2 productivity for PdAu/Si x Al.
研究领域:
催化
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
·
2021
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IF 5.876
Yanfang Chen,Xuemei Yan,Haifeng Lin,Chao Wang,Jixiang Xu
Background Fe 2+ /H 2 O 2 -based photo-Fenton process is often used in pollutions removal. But, Fe-species related low activity at neutral condition hinders their practical applications. Activation of in situ generated H 2 O 2 for Fenton-like degradation of pollutions through catalysts absences of Fe species is expected. Methods A strip-like benzene and K + co-doped g-C 3 N 4 (KBCN) was constructed by the thermal polymerization of assembly of melamine and 2-aminoterephthalic acid, then post-calcination in LiCl–KCl molten salt, which was then used to degrade Rhodamine B (RhB) and Congo red (CR) via in situ generated H 2 O 2 . Significant findings Benzene and K + co-doping were critical both in increasing charge separation and enhancing the H 2 O 2 production. The yield of H 2 O 2 for KBCN was 57.5 μM in pure water after 60 min irradiation. In the absence of Fe 2+ , the in situ generated H 2 O 2 could subsequently degrade RhB and CR with the formed ·OH. The apparent rate constants of KBCN for RhB and CR degradation were 0.0446 and 0.0497 min −1 , respectively. The advantages of degradation with in situ generated H 2 O 2 in the absence of Fe 2+ can provide a new prospective to the environmental friendly Fenton-like reaction.
研究领域:
环境科学
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Guiyang Yu,Ke Gong,Chuanwang Xing,Lan Hu,Haibin Huang,Lejie Gao,Debao Wang,Xiyou Li
Organic semiconductor under photoexcitation could generate abundant strong-binding Frenkel excitons and inevitably suffer from low dissociation efficiency (<1%) and poor mobility ability, which severely suppresses the efficient utilization of photogenerated charges and corresponding activity. Herein, a dual P-doping strategy is proposed in bay and corner sites implanted polymeric carbon nitride (PCN-D) for visible-driven H 2 O 2 production. The dual P doping breaks localized electron state around original symmetric heptazine units and weakens the binding energy between electrons and holes, increasing dissociation efficiency to reach 11.9% with 20-fold improvement. In addition, the conductivity ability of PCN-D, including formed carrier charge concentration and mobility, achieves 13-fold and 7-fold improvement, which facilitates the charge transfer and separation. The proposed dual doped-P-site strategy, with the blessing of porous structure, provides plentiful active center for effective adsorption and activation of O 2 molecule, further accelerating reaction progress and achieving six-times increase of photocatalytic H 2 O 2 production rate. This work provides in-depth insight into the importance of dual P-doping to optimize kinetic behavior of photogenerated charges and opens an avenue to the multiscale doping-modulation of semiconductor with high efficiency solar energy conversion.
研究领域:
材料科学
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化学
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光化学
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催化
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2024
·
IF 5.8
Haitao Li,Yingying Zhang,Han Dai,Veronica Pereir,Junfeng Zhao,Hiang Kwee Lee
Polyvinylidene fluoride (PVDF)-based piezoelectric catalysts show promise in mechanical force-driven catalysis due to their good biocompatibility, flexibility, and ease of fabrication. However, the catalytic activity of pristine PVDF is limited due to its low piezoelectric phase content (<20%), poor orientation, and low surface carrier concentration. Here, we introduce an efficient PVDF-based composite nano-catalyst (rGO/PVDF) with high piezoelectric catalytic performance. We achieve this by employing a composite strategy that combines nanoscale water-induced polarization with polar functional group-modified graphene (rGO) serving as a nanoelectrode. The nanoscale water polarization effect, together with the two-dimensional planar structure of PVDF and the modified graphene's polar functional groups, effectively induces orientation in the PVDF piezoelectric phase to increase the functional β phase content. As a result, the β phase content and crystallinity of rGO/PVDF reach 95% and 40%, respectively, which are 600% and 170% higher compared to those of pristine PVDF. This enhancement plays a crucial role in endowing the material with strong force-to-electricity conversion characteristics. Additionally, the surface-modified rGO also boosts PVDF's surface carrier concentration and provides active sites for catalysis on the rGO/PVDF composite. Notably, under optimized conditions, our catalyst achieves a ∼99.1% degradation rate of organic pollutants (10 mg L−1) after 12 minutes of sonication at 240 W and maintains a high efficiency of ∼93.7% even at a 10 times higher pollutant concentration (100 mg L−1). Our piezoelectric catalyst also demonstrates efficient H2O2 production at 95.8 mmol grGO−1 h−1, which is ∼9-fold and ∼134-fold higher than those of untreated PVDF and previously reported PVDF-based piezoelectric catalysts, respectively. This work paves the way for the development of highly efficient PVDF-based piezoelectric catalysts, thereby offering valuable insights for the advancement of mechanically driven catalysis in the environmental, energy, and chemical sectors.
研究领域:
材料科学
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环境科学
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催化
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纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Kailian Zhang,Man Zhou,Kai Yang,Changlin Yu,Ping Mu,Zhenzhen Yu,Kangqiang Lu,Weiya Huang,Wenxin Dai
The low-usage of solar energy and the sluggish separation efficiency of the photogenerated electrons/holes pairs are the obstacles in the practical application of photocatalysts. The integration of upconversion and Z-scheme heterojunction is expected to break the barriers to achieve the efficient charge separation and broaden near-infrared light absorption . Herein, an effective indirect Z scheme AgInS 2 /In 2 S 3 heterostructure with carbon quantum dots (CQDs, as the electron conduction medium) and Lu 3 NbO 7 :Yb, Ho (as upconversion function) has been successfully synthesized. Consequently, the Lu 3 NbO 7 : Yb, Ho/CQDs/AgInS 2 /In 2 S 3 heterostructure exhibited superior photocatalytic activities for Cr(VI) reduction and H 2 O 2 production, reducing 99.9% of Cr(VI)(20 ppm, 15 min) and 78.5% of Cr(VI) (40 ppm, 30 min) with visible light irradiation as well as 94.0% of Cr(VI) (20 ppm, 39 min) under NIR light irradiation. Simultaneously, the heterostructure could generate 902.9 μM H 2 O 2 for 5 h under visible light irradiation. The intensive photocatalytic properties could primarily be attributed to the boosted light absorption capacity, the improved solar-to-energy conversion by the remarkable upconversion capacity of Lu 3 NbO 7 : Yb, Ho/CQDs and the faster charge transfer through a Z-schematic pathway. This work is anticipated to open a novel “window” for designing the efficient photocatalysts by coupling of Lu 3 NbO 7 : Yb, Ho and CQDs.
研究领域:
材料科学
·
环境科学
·
光化学
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）