4.8 Article

PdS Quantum Dots as a Hole Attractor Encapsulated into the MOF@Cd0.5Zn0.5S Heterostructure for Boosting Photocatalytic Hydrogen Evolution under Visible Light

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume -, Issue -, Pages -

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c15052

Keywords

photocatalysis; hydrogen evolution; metal-organic framework; quantum dot; heterojunction; co-catalyst

Funding

  1. National Natural Science Foundation of China [21972110, 51702253]
  2. State Key Laboratory of Electrical Insulation and Power Equipment [EIPE23315]

Ask authors/readers for more resources

A new photocatalyst PdS@UiOS@CZS with excellent photocatalytic H-2 evolution rate is successfully synthesized by encapsulating PdS quantum dots in thiol-functionalized UiO-66 and anchoring Cd0.5Zn0.5S solid solution nanoparticles on its outer surface. The significantly enhanced performance is attributed to the attraction of photogenerated holes by encapsulated PdS QDs into the pores of UiOS and the effective migration of photogenerated electrons to CZS due to the heterojunction effect, thereby suppressing the recombination of charge carriers.
Herein, a new photocatalyst PdS@UiOS@CZS is successfully synthesized, where thiol-functionalized UiO-66 (UiOS), a metal-organic framework (MOF) material, is used as a host to encapsulate PdS quantum dots (QDs) in its cages, and Cd0.5Zn0.5S (CZS) solid solution nanoparticles (NPs) are anchored on its outer surface. The resultant PdS@UiOS@CZS with an optimal ratio between components displays an excellent photocatalytic H-2 evolution rate of 46.1 mmol h(-1) g(-1) under visible light irradiation (420 similar to 780 nm), which is 512.0, 9.2, and 5.9 times that of pure UiOS, CZS, and UiOS@CZS, respectively. The reason for the significantly enhanced performance is that the encapsulated PdS QDs strongly attract the photogenerated holes into the pores of UiOS, while the photogenerated electrons are effectively migrated to CZS due to the heterojunction effect, thereby effectively suppressing the recombination of charge carriers for further high-efficiency hydrogen production. This work provides an idea for developing efficient photocatalysts induced by hole attraction.

Authors

I am an author on this paper
Click your name to claim this paper and add it to your profile.

Reviews

Primary Rating

4.8
Not enough ratings

Secondary Ratings

Novelty
-
Significance
-
Scientific rigor
-
Rate this paper

Recommended

Article Engineering, Electrical & Electronic

BaTiO3-Refined NiCuZn Ferrites Towards Enhanced Pulse Detection Sensitivity for a High-Frequency Current Transformer

Sen Qian, Chuan Chen, Yan Wang, Hongkang Wang

Summary: This research focuses on improving the sensitivity of High-frequency current transformer (HFCT) sensors for pulse detection at high frequencies by refining the ferrites of the magnetic cores. The results show that the use of a two-step sintering technique and the addition of barium titanate (BaTiO3) can significantly improve the transfer functions of the HFCT sensors, thereby enhancing their sensitivity for pulse detection at high frequencies.

JOURNAL OF ELECTRONIC MATERIALS (2023)

Article Nanoscience & Nanotechnology

Rational Regulation of Reducibility and Acid Site on Mn-Fe-BTC to Achieve High Low-Temperature Catalytic Denitration Performance

Kunli Song, Kaiyu Guo, Yixuan Lv, Dandan Ma, Yonghong Cheng, Jian-Wen Shi

Summary: Selective catalytic reduction with ammonia is the mainstream technology for flue gas denitration. The reducibility and acid site are two important factors affecting de-NOx performance, and their regulation through synthesis of Mn-Fe-BTC catalyst with different ratios of Mn and Fe has been investigated. The research provides guidance for flexible regulation of reducibility and acid site of low-temperature de-NOx catalyst.

ACS APPLIED MATERIALS & INTERFACES (2023)

Article Chemistry, Multidisciplinary

Embedding antimony nanoparticles into metal-organic framework derived TiO2 @carbon nanotablets for high-performance sodium storage

Tianhao Yao, Li Li, Hongkang Wang

Summary: Titanium dioxide has been extensively studied as anode materials for sodium-ion batteries due to its low cost and high abundance. However, its slow ion/electron transfer rate limits its practical applications. In this study, TiO2@C-Sb nanotablets with a small amount of Sb content were developed through calcination of Ti-metal-organic framework derived TiO2@C/SbCl3 mixture. The TiO2@C-Sb exhibits enhanced electron/ion transfer rate and predominantly pseudocapacitive sodium storage behavior, making it a promising candidate for high-energy-density TiO2-based energy storage devices.

CHINESE CHEMICAL LETTERS (2023)

Article Chemistry, Physical

Graphitic carbon nitride decorated with C-N compounds broken by s-triazine unit as homojunction for photocatalytic H2 evolution

Yixuan Lv, Dandan Ma, Kunli Song, Siman Mao, Zhetong Liu, Dan He, Xuewen Zhao, Tianhao Yao, Jian-Wen Shi

Summary: The gradual depletion of global fossil energy and environmental pollution make the development of hydrogen energy an imminent concern. Researchers have found that introducing broken C-N compounds to construct homojunctions on two-dimensional g-C3N4 can significantly enhance photocatalytic H-2 generation and effectively suppress the recombination of photogenerated electrons and holes.

JOURNAL OF MATERIALS CHEMISTRY A (2023)

Article Chemistry, Multidisciplinary

Insights into the Role of Graphitic Carbon Nitride as a Photobase in Proton-Coupled Electron Transfer in (sp3)C-H Oxygenation of Oxazolidinones

Alexey Galushchinskiy, Yajun Zou, Jokotadeola Odutola, Pavle Nikacevic, Jian-Wen Shi, Nikolai Tkachenko, Nuria Lopez, Pau Farras, Oleksandr Savateev

Summary: Graphitic carbon nitride (g-CN) is a transition metal free semiconductor that mediates photocatalytic reactions through proton-coupled electron transfer (PCET) mechanism. The active sites for PCET are identified as the 'triangular pockets' on the edge facets of g-CN. Using excited state PCET, g-CN can selectively cleave X-H bonds with approximately 100 kcal mol(-1) bond dissociation free energy (BDFE), leading to the formation of 1,3-oxazolidine-2,4-diones.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2023)

Article Engineering, Multidisciplinary

Enhancing pseudocapacitive behavior of MOF-derived TiO2-x@Carbon nanocubes via Mo-doping for high-performance sodium-ion capacitors

Tianhao Yao, Hongkang Wang, Yuanbin Qin, Jian-Wen Shi, Yonghong Cheng

Summary: This study presents a novel approach to enhance the storage behavior and reaction kinetics of TiO2-based anode in sodium-ion capacitors (SICs) through Mo-doping and carbon hybridization. The Mo-doped TiO2-x@carbon composite exhibits improved pseudocapacitive contribution, reversible capacity, cycling stability, and rate capability.

COMPOSITES PART B-ENGINEERING (2023)

Article Materials Science, Multidisciplinary

Construction of PdS@MIL-125-NH2 @ZnS type-II heterostructure with efficient charge separation for boosted photocatalytic hydrogen evolution

Zige Tai, Guotai Sun, Ting Wang, Zhihui Li, Jinge Tai

Summary: For the first time, a new photocatalyst PdS@NH2-MIL-125(Ti)@ZnS (PdS/M125/ZnS) heterojunction was fabricated for photo-catalytic H2 generation. The optimized photocatalyst displayed a significantly enhanced H2 generation rate compared to pure M125, attributed to the hierarchical structure and the type-II heterojunction formed by M125, ZnS, and PdS co-catalyst. This work provides a new avenue for designing MOFs photocatalysts for energy conversion.

JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY (2023)

Article Chemistry, Multidisciplinary

Introducing Hybrid Defects of Silicon Doping and Oxygen Vacancies into MOF-Derived TiO2-X@Carbon Nanotablets Toward High-Performance Sodium-Ion Storage

Tianhao Yao, Hongkang Wang, Xin Ji, Deyu Wang, Qingmiao Zhang, Lingjie Meng, Jian-Wen Shi, Xiaogang Han, Yonghong Cheng

Summary: Titanium dioxide (TiO2) is a promising anode material for sodium-ion batteries (SIBs) but suffers from slow ion transferability and poor conductivity. To overcome these drawbacks, a facile strategy has been developed to engineer the lattice defects and microstructure of TiO2-based anode, resulting in enhanced sodium storage performance.

SMALL (2023)

Article Chemistry, Physical

Insight into the Origin of Excellent SO2 Tolerance and de-NOx Performance of quasi-Mn-BTC in the Low-Temperature Catalytic Reduction of Nitrogen Oxide

Kunli Song, Kaiyu Guo, Siman Mao, Dandan Ma, Yixuan Lv, Chi He, Hongkang Wang, Yonghong Cheng, Jian-Wen Shi

Summary: This study reports a selective catalytic reduction (SCR) catalyst, quasi-metal-organic-framework (MOF) nanorod containing manganese (quasi-Mn-BTC),which overcomes the disadvantage of poor SO2 tolerance of Mn-based catalysts. The catalyst exhibits excellent low-temperature (LT) denitration (de-NOx) performance and maintains high NOx conversion even under high SO2 concentration.

ACS CATALYSIS (2023)

Article Chemistry, Multidisciplinary

Noble-Metal-Free Ultrathin CdS-NiFeS 2D-2D Heterojunction Nanosheets for Significantly Enhanced Photocatalytic Hydrogen Evolution

Guotai Sun, Zige Tai, Fan Li, Qian Ye, Ting Wang, Zhiyu Fang, Xiaoxiong Hou, Lichao Jia, Hongqiang Wang

Summary: To effectively reduce the charge recombination of bulk CdS, this study designed ultrathin CdS-NiFeS 2D-2D heterojunctions with tight interfaces, in which NiFeS nanosheets derived from layered double hydroxides have tunable work functions and hydrogen evolution overpotentials. The optimized CdS-2% NiFe0.1S photocatalyst exhibits excellent hydrogen generation activity, reaching 626.7 mu mol/h (equivalent to 62.67 mmol/g/h), which is highly competitive among noble-metal-free CdS-based catalysts. The enhanced catalytic performance is attributed to the establishment of sufficient contact interfaces, the shortened charge transport distance, and efficient electron transfer from CdS to NiFeS, as well as the presence of the bimetallic NiFeS cocatalyst providing abundant active sites and lowering the reaction barrier for H2 generation. This research provides new insights for the development of 2D nanomaterials with outstanding photocatalytic performance.

ACS SUSTAINABLE CHEMISTRY & ENGINEERING (2023)

Article Energy & Fuels

MnyCo3_ yOx bimetallic oxide prepared by ultrasonic technology for significantly improved catalytic performance in the reduction of NOx with NH3

Xiangbo Feng, Baorui Wang, Ge Gao, Shan Gao, Chong Xie, Jian-Wen Shi

Summary: In this study, a series of Mn-Co mixed metal oxides (MnyCo3_yOx) were prepared using ultrasonic technology and hydrothermal treatment, and their denitration performance in selective catalytic reduction (SCR) with NH3 was evaluated. The results showed that MnyCo3_yOx had significantly better SCR de-NOx performance compared to single metal oxides (MnOx or CoOx). This improvement was attributed to the strong interaction between MnOx and CoOx, which reduced crystallinity, increased surface area, facilitated redox cycling, enhanced reducibility and surface acid sites, and accelerated the reaction between adsorbed NOx species and coordinated NH3. This work suggests that building a strong interaction between catalyst components can improve de-NOx performance.
Article Chemistry, Multidisciplinary

Anatase/Rutile Phases Regulating TiO2/C Heterointerfaces for Enhanced Polysulfide Conversion in Sulfur Cathodes

Chong Xie, Na Xu, Zhenyu Wang, Yixuan Lv, Ruixian Duan, Guiqiang Cao, Wei Xiao, Jian Qin, Jian-Wen Shi, Jiujun Zhang, Xifei Li

Summary: Designing heterostructured hosts is crucial for enhancing the performance of lithium-sulfur batteries. In this study, ultrafine anatase and rutile TiO2 nanoparticle-modified macroporous carbon microspheres were synthesized. The TiO2/C heterointerfaces constructed by anatase TiO2 demonstrated a higher catalytic efficiency compared to rutile TiO2, leading to a high specific capacity and low capacity decay rate for the S@AT@MC electrodes.

ACS SUSTAINABLE CHEMISTRY & ENGINEERING (2023)

Article Chemistry, Physical

Construction of II-type and Z-scheme binding structure in P-doped graphitic carbon nitride loaded with ZnO and ZnTCPP boosting photocatalytic hydrogen evolution

Xuan Xu, Xiangbo Feng, Wei Wang, Kunli Song, Dandan Ma, Yixuan Zhou, Jian-Wen Shi

Summary: A ternary heterostructure (ZnPPO) consisting of ZnO, tetrakis (4-carboxyphenyl) zinc porphyrin (ZnTCPP), and P-doped g-C3N4 (PCN) was developed. ZnPPO demonstrates superior photocatalytic activity for H2 generation from water splitting compared to binary heterostructures and single components. The enhancement can be attributed to the effective transfer of photo-generated charge carriers in the II-type and Z-scheme binding structure.

JOURNAL OF COLLOID AND INTERFACE SCIENCE (2023)

Article Chemistry, Physical

Low-temperature selective catalytic reduction of NOx with NH3: Exploring the mechanism of enhancing H2O tolerance through methylation functionalization and structural regulation in IPAx-Mn-BTC

Kunli Song, Jiyuan Hu, Peng Lu, Dandan Ma, Xinya Zhou, Jun Li, Ting Jiang, Lu Li, Shangyuan Wu, Jian-Wen Shi

Summary: In this study, a low-temperature de-NOx catalyst with strong H2O tolerance was developed through methyl functionalization. The catalyst showed only a slight decrease in NOx conversion when 6% H2O was introduced at low temperature. The elimination of small pore size and diminished H2O adsorption energy due to methyl functionalization were found to be the key factors behind the improved H2O tolerance.

APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY (2024)

Article Materials Science, Multidisciplinary

Yolk-shelled LiNi0.6Co0.2Mn0.2O2 cathode for high-performance lithium ion batteries: a general synthetic strategy

Ang Gao, Tianhao Yao, Menglong Yao, Ruochen Chen, Qiangrui He, Hongkang Wang

Summary: By complexing Ni/Co/Mn ions with glucose under solvothermal conditions, well-defined spherical Ni/Co/Mn-gluconate with tunable size and elemental composition is prepared and can be readily converted into yolk-shelled Li(NixCoyMn1-x-y)O-2. A yolk-shelled LiNi0.6Co0.2Mn0.2O2 cathode is prepared as an example and exhibits high specific lithium storage capacity and excellent cycling stability.

MATERIALS ADVANCES (2023)

No Data Available