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Solar RRL · 2020 ·Vol. 5 ·期 6 ·2000427 · IF 7.527

Engineering of 2D/2D MoS2/CdxZn1−xS Photocatalyst for Solar H2 Evolution Coupled with Degradation of Plastic in Alkaline Solution

Yiqun Li,Shipeng Wan,Cheng Lin,Yujie Gao,Yuan Lu,Luyang Wang,Kan Zhang

Sufficiently utilizing photogenerated electron/hole pairs for a coupled redox enables green, sustainable, and low-cost photocatalysis. Herein, a series of MoS 2 /Cd x Zn 1− x S photocatalysts with uniform 2D/2D structure are reported for solar water–reductive H 2 products coupled with the degradation of polyethylene terephthalate (PET) plastic. The MoS 2 /Cd 0.5 Zn 0.5 S heterojunction with a loading mass of 4.3 wt% MoS 2 exhibits the best H 2 evolution rate of 15.90 mmol g −1 h −1 in an aqueous solution due to its appropriate redox ability, great light absorption, and carrier separation abilities. Then, the oxidation products of PET are analyzed by 1 H-NMR spectroscopy, which demonstrates the PET being efficiently degraded to molecule compounds, such as formate and acetate. The work provides a feasible solution to the problem of plastic pollution and meets the demand for sustainable clean energy simultaneously.

研究领域: 材料科学 · 环境科学 · 能源科学 · 化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2020 · IF 4.939

Well-defined FeP/CdS heterostructure construction with the assistance of amine for the efficient H2 evolution under visible light irradiation

Ming-Yu Dou,Shu-Rui Han,Xin-Xin Du,Dong-Hui Pang,Lei-Lei Li

The photocatalyst is a crucial factor in determining solar-to-H 2 efficiency for solar-driven water splitting. Here, the FeP/CdS well-defined heterostructure was elaborately designed and successfully constructed in-situ to achieve efficient water splitting by using a simple and green solvothermal approach. In the synthetic process, the ethylenediamine plays an important role in the construction of intimate contact interface between FeP and CdS. This good quality FeP/CdS heterostructure can efficiently promote charge separation and transportation, and therefore the charge recombination of CdS was significantly suppressed. As a result, the as-synthesized FeP/CdS heterostructure showed excellent photocatalytic performance under visible-light irradiation with an optimal hydrogen evolution rate of 37.92 mmol g −1  h −1 and an apparent quantum yield of 31.50% at 420 nm far exceeding that of pristine CdS by more than 122 folds. This rate, to the best of our knowledge, outperforms other similar catalytic systems .

研究领域: 材料科学 · 能源科学 · 化学工程
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Nano Select · 2021 ·Vol. 2 ·期 11 ·2126-2134 · IF 0

Stable Pt atomic clusters on carbon nanotubes grafted with carbon quantum dots as electrocatalyst for H2 evolution in acidic electrolyte

Junwei Liang,Yuxiang Liu,Rongzheng Liu,Sufan Zheng,Zhichun Si,Duan Weng,Feiyu Kang

Preparing stable highly dispersed Pt based electrocatalyst is promising to reduce material expense of H 2 product via electrocatalytic water splitting. However, it is still a great challenge to obtain stable single atomic Pt catalysts which can be applied in acidic electrolyte. In the present work, we synthesized Pt atomic clusters on carbon quantum dots (CQDs) grafting multiwall carbon nanotube (CNT) (Pt content: 1 wt.%) catalysts and then loading the catalysts on carbon cloth (Pt content: 0.01 mg▪cm –2 ) for activity test. The overpotential of 29 mV versus RHE was obtained over 1%Pt/CQDs/CNT catalysts at the current density of 10 mA▪cm –2 , and the Tafel slope of 22 mV decade –1 was obtained, too. Especially, the catalysts showed significant stability in hydrogen evolution reactions (HER) in acidic solution, of which the overpotential was still smaller than that of 20%Pt/C after 10,000 CV cycles. CQDs provided coordinating sites for dispersing Pt atomic clusters and improved the H + concentration in adjacent area around the Pt clusters. This method provides a general strategy to design the highly efficient electrocatalysts with ultra-low precious metals for H 2 evolution in acidic electrolyte.

研究领域: 材料科学 · 电化学 · 纳米技术 · 能量转换 · 催化
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

In-situ preparation of mossy tile-like ZnIn2S4/Cu2MoS4 S-scheme heterojunction for efficient photocatalytic H2 evolution under visible light

Shikai Wang,Dafeng Zhang,Ping Su,Xintong Yao,Junchang Liu,Xipeng Pu,Hengshuai Li,Peiqing Cai

The reasonable design and fabrication of heterojunction could regulate the photocatalytic performance to some extent, yet it is still a great challenge to construct the S-scheme heterostructure with the stable as well as tight interface on the surface of semiconductor photocatalysts. Herein, the ZnIn 2 S 4 /Cu 2 MoS 4 (ZIS/CMS) S-scheme heterostructure was fabricated by in-situ assembling ZIS nanosheets on the CMS plates, obtaining a mossy tile-like morphology. Owing to the compact interface resulting from in-situ growth, this unique architecture efficiently facilitated the separation and transfer of light-induced charges, guaranteed the larger interface area, and enriched the active sites for photocatalytic redox reactions. After adjusting the mass ratio of CMS in ZIS/CMS, S-scheme heterostructure exhibited the remarkable performance with an optimal H 2 producing rate up to 1298 μmol·h −1 g −1 , about 13.8 times than that of pristine ZIS. The mechanism and driving force of charge transfer and separation in S-scheme heterostructure photocatalysts were explained and discussed. This investigation will provide new insight into design and construction of S-scheme heterojunction photocatalysts for H 2 evolution.

研究领域: 材料科学 · 能源化学
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APPLIED ENERGY · 2024 · IF 10.1

Ultra-rapid formation of mixed H2/DIOX/THF hydrate under low driving force: Important insight for hydrate-based hydrogen storage

Yaning Kong,Honglin Yu,Mengqi Liu,Guodong Zhang,Fei Wang

Hydrate was considered to be the next generation hydrogen storage material , and hydrate-based hydrogen storage (HBHS) would play an important role in future hydrogen economy, but sluggish hydrate formation kinetics presents huge technological challenge for its application. Herein, a nano promoter of -SO 3 − @PSNS was prepared by soap-free emulsion polymerization , and a dual kinetic promoter system (L-methionine/-SO 3 − @PSNS) was applied to enhance the formation kinetics of mixed H 2 /DIOX hydrate. At a moderate condition (12 MPa and 274.15 K), hydration efficiency under a driving force of 2.1 MPa is significantly enhanced by the synergy of the dual kinetic promoters, hydrate induction time reduces from 443.2 ± 209.73 min to 24.7 ± 17.16 min, while hydrate growth rate increases by 43.75%, and hydrogen storage capacity is up to 0.473 ± 0.041 wt% that increases by 62.8%. At a more moderate condition (10 MPa and 274.15 K) with an extremely low driving force of 0.1 MPa, enhanced hydrate formation was obtained in a composite promotion system of the dual kinetic promoters and dual thermodynamic promoters (THF/DIOX), which also performs exceptionally in term of recycling. The presence of a small amount (0.35 mol%) of THF reduces the induction time by 93.5%, and hydrate growth rate increases by 130.18%, while satisfactory hydrogen storage capacity (0.346 ± 0.017 g/g) is still remained in mixed H 2 /DIOX/THF hydrate, the structure of which was confirmed by Raman spectrum . This work presents an effect approach on enhancing the formation kinetics of H 2 -contained hydrate under low driving force, and this finding provides important insight for HBHS.

研究领域: 物理化学 · 能源材料 · 气体储存 · 化学工程 · 纳米材料科学 · 分子模拟 · 可持续能源
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

C, N-vacancies and Br dopant co-enhanced photocatalytic H2 evolution of g-C3N4 from water and simulated seawater splitting

Mingrui Guo,Meng Chen,Jixiang Xu,Chao Wang,Lei Wang

Introducing defects and heteroatoms on carbon nitride (g-C 3 N 4 , CN) framework are effective ways to enhance its photocatalytic activity by regulating light absorption and charge carriers separation. Herein, a mechanochemical method was employed to synthesize Br-doped C, N-deficient CN (CN V -mCN-Br) via ball-milling of N-containing precursor and 6-Bromopyridine-3-carbaldehyde (BrPyCHO) followed by calcining. The ball-milling-evolved mechanical forces and BrPyCHO-derived HBr induced formation of C, N vacancies and C-Br bond in CN V -mCN-Br framework. The CN V -mCN-Br exhibited curled nanosheets morphology and separated electrons-holes distribution. The photocatalytic H 2 evolution rates of 1 %Pt-loaded CN V -mCN-Br in distilled water and simulated seawater were 22.21 and 34.41 mmol g –1 h −1 , respectively with 10% triethanolamine . The corresponding apparent quantum yields were 25.87% and 40.08% at 420 nm. This work provides a facile technique to simultaneously introduce defect and heteroatom in CN for high-efficiency photocatalytic H 2 evolution.

CAS / MDL: 108-80-5 108-78-1
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Novel noble-metal-free Co2P/CdIn2S4 heterojunction photocatalysts for elevated photocatalytic H2 production: Light absorption, charge separation and active site

Xiaohui Ma,Wenjun Li,Hongda Li,Mei Dong,Liang Geng,Tianyu Wang,Hualei Zhou,Yanyan Li,Mengchao Li

Constructing heterojunctions is an effective and controllable approach that can boost the activity of photocatalysts. Inspiringly, this study explored a simple method that can be used to construct novel noble-metal-free Co 2 P/CdIn 2 S 4 (CPCIS) heterojunction photocatalysts for photocatalytic hydrogen production. The heterojunction was formed by loading CdIn 2 S 4 (CIS) nanoparticles on the surface of Co 2 P (CP). The structure, morphology, and optical property of the as-prepared samples were characterized by a series of tests. The DRS results showed that, the light absorption range of CPCIS was extended to the full visible light range and its light absorption intensity obviously was enhanced at 500–800 nm. The PL and photoelectrochemical tests manifested that the formed heterojunction promoted the separation of charges. The LSV results indicated that CP reduced the H 2 evolution overpotential of the composites. Besides, CP could serve as active sites of H 2 evolution in heterojunction composites. Interestingly, the H 2 -evolution rate for the optimum CPCIS (471.87 μmol h −1 g −1 ) was around 3.6 times than CIS-Pt. The elevated activity of CPCIS may mainly attribute to the following aspects: its enhanced light absorption, elevated charge separation and increased active site. More importantly, the photocatalytic activity of heterojunction composites didn’t almost decrease after three cycles. This article delivers an idea that can be applied to form heterojunctions between CP and other sulfides for photocatalytic H 2 production, easily extending to other transition metal phosphides.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Interfacial intimacy and internal electric field modulated S-scheme Sv-ZnS/ZnIn2S4 photocatalyst for efficient H2 evolution and CO2 reduction

Jingyuan Liu,Min Liu,Subin Zheng,Xiaoyang Liu,Shunyu Yao,Fengyang Jing,Gang Chen

The construction of S-scheme heterojunctions is an effective approach to realize artificial photocatalytic processes. For the higher solar energy conversion efficiency, current research focuses on improving the interfacial intimacy and precisely modulating the strength of the internal electric field (IEF). To address this issue, we propose a novel MOF-based synthesis and derivation strategy. The heterojunction obtained by this strategy tends to form an intimate interface and a tunable IEF, which facilitates the transfer and separation of photogenerated carriers. Herein, a ZnS/ZnIn 2 S 4 (ZIS) S-Scheme heterojunction containing sulfur vacancies (Sv) was successfully synthesized, and its good photocatalytic hydrogen evolution reaction (HER) and CO 2 reduction reaction (CO 2 RR) activity confirmed the feasibility of this strategy. The prepared Sv-ZnS/ZIS exhibits an apparent quantum yield of 19.8 ± 1.0 % at 420 nm and a hydrogen evolution rate of 2912.3 ± 185.9 μmol g −1 h −1 , which is 9.0 and 33.6 times higher than pure ZIS and Sv-ZnS, respectively. Furthermore, the yield of photoreduction CO 2 to CO reaches 2075.7 ± 63.0 μmol g −1 h −1 with a CO selectivity of 93.0 ± 0.8 %. This work provides new sights for the rational design and construction of S-scheme photocatalysts with sulfur vacancies for efficient photocatalysis.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

K–N Bridge-Mediated charge separation in hollow g-C3N4 Frameworks: A bifunctional photocatalysts towards efficient H2 and H2O2 production

Xiaoli Jin,Huiqing Wang,Xiongtao Lv,Qing Lan,Teng Ge,Lin Guo,Xin Li,Hongxian Sun,Chenghua Ding,Yuwei Guo,Haiquan Xie,Liqun Ye

The development of bifunctional photocatalysts for enhancing hydrogen (H 2 ) and hydrogen peroxide (H 2 O 2 ) production from water is essential in addressing environmental and energy issues. However, the practical implementation of photocatalytic technology is still constrained by the inadequate separation of photo-generated charge carriers. Herein, potassium (K) atoms are introduced into the interlayers of graphitic carbon nitride (g-C 3 N 4 ) with a hollow hexagonal structure (K-TCN) and are coordinated with N atoms in adjacent layers. The presence of K–N coordination serves as a layer bridge, facilitating the separation of charge carriers. The hollow hexagonal structure reduces the distance over which photogenerated electrons migrate to the surface, thereby enhancing the reaction kinetics. Consequently, the optimized K-TCN exhibits a dramatically improved photocatalytic H 2 (941.6 μmol g −1 h −1 with platinum (Pt) as the cocatalyst) and H 2 O 2 (347.6 μmol g −1 h −1 ) generation as compared to hollow g-C 3 N 4 (TCN) and bulk g-C 3 N 4 nanosheet (CN) without K–N bridge under visible light irradiation. The unique design holds promising potential for developing highly efficient bifunctional photocatalysts towards producing renewable fuels and value-added chemicals.

CAS / MDL: 461-58-5
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CHEMICAL ENGINEERING SCIENCE · 2023 · IF 4.7

On-the-fly H2 degassing: Towards selective borohydride reduction of α, β-unsaturated esters to allylic alcohols in continuous microflow

Jiale Wu,Yuan Tao,Dang Cheng,Fener Chen

Herein, we demonstrate a hybrid microflow system consisting of a coaxial double-tube microreactor and a capillary microreactor for performing borohydride reduction of α , β -unsaturated esters to allylic alcohols in a highly controlled and safe manner. Using methyl cinnamate as the model substrate and LiBH 4 as reductant, complete conversion was achieved in 75 s residence time at 80 ℃ with up to 85% yield of the target product cinnamyl alcohol under optimized conditions in the hybrid microflow system, enabling selective borohydride reduction of α , β -unsaturated esters to allylic alcohols without the need of using metallic salts as additives or co-reagents. The kinetics of this reduction reaction has been examined and modelled, providing an understanding of the intensified reaction behaviour and the reaction performance of the hybrid microflow process. The results presented can shed new light on the development of continuous microflow processes for the hydridic type of reductions.

CAS / MDL: 104-55-2
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Anchoring Bi2S3 quantum dots on flower-like TiO2 nanostructures to boost photoredox coupling of H2 evolution and oxidative organic transformation

Bing Xing,Ting Wang,Xiaobo Han,Kun Zhang,Benxia Li

The rational integration of semiconductor quantum dots (QDs) with anatase TiO 2 nanostructures is a promising strategy to develop efficient photocatalysts. Herein, Bi 2 S 3 QD/TiO 2 photocatalyst was constructed by controllably depositing Bi 2 S 3 QDs on flower-like TiO 2 nanostructures and used for the photocatalytic redox-coupling reaction of H 2 evolution and oxidative transformation of benzyl alcohol. The abundant amino groups in TiO 2 nanostructures served as the anchoring sites for uniform growth of Bi 2 S 3 QDs. The anchoring of Bi 2 S 3 QDs onto TiO 2 nanostructures not only enhanced the photoabsorption ability and the photogenerated charge separation efficiency but also afforded powerful photogenerated charge carriers and abundant active sites for the photocatalytic reaction. As a result, the Bi 2 S 3 QD/TiO 2 photocatalyst exhibited a favorable performance in the redox-coupling reaction, providing the high production rates of H 2 up to 4.75 mmol·g cat −1 ·h −1 and benzaldehyde up to 6.12 mmol·g cat −1 ·h −1 , respectively, as well as an excellent stability in the long-term photocatalytic reaction. Meanwhile, a trace amount of water in the reaction system could act as a promoter to accelerate the photocatalytic redox-coupling reaction. The photocatalytic mechanism following S-scheme heterojunction was proposed according to the systematic characterizations and experimental results. This work offers some insight into the rational construction of efficient and cost-effective photocatalysts for the conversion of solar to chemical energy.

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Journal of Materials Chemistry A · 2022 ·Vol. 11 ·期 1 ·178-186 · IF 14.511

Bifunctional carbon dots as cocatalyst and reactor decorating an organic photocatalyst for H2 production from water-splitting in an emulsion

Zhenyu Wu,Qiang Hong,Xiting Wang,Hong Shi,Tianyang Zhang,Yu Zhao,Hui Huang,Yang Liu,Zhenhui Kang

Generation of clean hydrogen (H2) energy by photocatalytic water-splitting is a prospective method for solving the global energy crisis and environmental pollution and the design of new generation catalysts is expected to combine the functions of catalysis and reactor. Here, we illustrate the synthesis of organic polymer photocatalyst p(DB) synthesized from 5,11-dihydroindolo[3,2-b]carbazole and 1,2-bis(4-bromophenyl)ethane. The carbon dots (CDs) are utilized to modify p(DB) and the optimal sample 5% CDs/p(DB) exhibits highly efficient H2 production under visible light in an o-xylene-in-water emulsion, whose average rate of H2 evolution reaches 140.88 μmol g−1 h−1. Furthermore, the transient photovoltage (TPV) and photoelectrochemical measurements suggest that the CDs improve the charge transfer process and the charge extraction ability of p(DB). Moreover, the CDs play the role of an emulsifying agent as well as providing chemical reaction sites for photocatalytic water-splitting. This work provides a deep understanding of the functions of CDs to integrate a cocatalyst and reactor.

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