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·
2022
·Vol. 18
·期 32
·2203020
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IF 15.153
Kai Deng,Wenxin Wang,Qiqi Mao,Hongjie Yu,Ziqiang Wang,You Xu,Xiaonian Li,Hongjing Wang,Liang Wang
Tailoring the morphology and crystal structure of metallene is critical to improve its electrocatalytic performance. In this work, hetero-phase RhB metallene ( h -RhB metallene) with amorphous/crystalline structure is readily prepared by a two-step method. The h -RhB metallene is very unique in its non-metallic heteroatom doping and amorphous/crystalline structure. Benefiting from the unique metallene structure and the optimized electronic states induced by the incorporation of B atoms, the h -RhB metallene exhibits superior performance for hydrogen evolution reaction and hydrogen peroxide electro-oxidation reaction (HPOR). When coupled with HPOR, the h -RhB metallene|| h -RhB metallene water electrolysis two-electrode system exhibits a lower cell voltage of 0.379 V (@ 10 mA cm −2 ) compared with the overall water splitting (1.35 V). The presented synthetic method provides a powerful strategy to design metallene with hetero-phase for energy-saving H 2 production.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Li Luo,Jinfeng Tian,Wenfeng Hu,Peng Han,Wei Wang,Baojun Ma
Non-noble metal co-catalysts for hydrogen production have capacitance characterization, which can store photo-excited electrons from semiconductor and show capacitance catalysis. However, the overlarge capacitance of co-catalysts constrains prompt release of electrons. Here, we reported a new and highly efficient co-catalyst Zn-Ni 5 P 4 via evenly doping Zn in Ni 5 P 4 . Loading Zn-Ni 5 P 4 on CdS, the photocatalyst Zn-Ni 5 P 4 /CdS shows an ultrahigh activity of 8969 μmol/g/h, which is 2.4 times of Ni 5 P 4 /CdS (3668 μmol/g/h). More interestingly, by the Pt loading on the surface of Ni 5 P 4 , the (Pt/Ni 5 P 4 )/CdS shows only 1.3 times of Ni 5 P 4 /CdS. Zn doping in Ni 5 P 4 reduces the capacitance by 140 mF/g and electrochemical impedance, which benefits the release of photo-excited electrons. Moreover, the reduced overpotential and the increased specific surface area also account for the enhanced co-catalytic performance of Zn-Ni 5 P 4 . This paper presents an effective and low-cost method to inhibit negative effect of capacitance catalysis of non noble co-catalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Manyi Gao,Weiwei Yang,Yongsheng Yu,Jiaming Li,Yequn Liu
Plasmonic Au-mediated polymeric carbon nitride (PCN) has been recognized as one of the promising materials for photocatalytic applications due to its excellent properties in wide visible light spectrum, however it is still hindered by low catalytic efficiency. In this work, it was established that strong metal-support interactions (MSI) at the interface between plasmonic Au nanoparticles (NPs) and PCN nanosheets (PCNS) improves its photocatalytic efficiency. The resulting Au/PCNS 2.5 exhibits excellent photocatalytic activity with H 2 evolution rate up to 4.84 mmol g -1 h -1 under visible light, 12.4 times higher than that of bulk PCN. Such strong MSI significantly strengthens the localized surface plasmon resonance (LSPR) effect of Au NPs and the charge “pump” role of Schottky junctions at Au-PCNS interface, resulting in broad light absorption range as well as effective separation and transfer of charge carrier. This work provides a new way to design the plasmonic photocatalysts for splitting water as well as other plasmon-driven chemical reactions.
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Journal of Environmental Sciences
·
2021
·
IF 5.565
Weilai Wang,Fan Zhang,Yunfei Zhang,Lei Xu,Yuansheng Pei,Junfeng Niu
Hydrodechlorination is a promising technology for the remediation of water body contaminated with trichloroethylene (TCE). In this work, the liquid-phase hydrogenation of TCE by Raney Ni (R-Ni) and Pd/C under an open system have been studied, in which nascent H 2 (Nas-H 2 ) generated in situ from the cathode acted as a hydrogen source. Experimental results showed that TCE was completely eliminate from the solution through the synergistic effects of hydrodechlorination and air flotation due to the formation of continuous micro/nano-sized Nas-H 2 bubbles from the cathode. Furthermore, the effects of inorganic anions and organic solvents on R-Ni and Pd/C hydrogenation activity were investigated, respectively. The results showed that NO 3 − and acetonitrile can form a competitive reaction with TCE; Sulfur with lone-pair electrons will cause irreversible poisoning to these two catalysts, and have a stronger inhibitory effect on Pd/C. This work helps to realize the separation of volatile halogenated compounds from water environment and provides certain data support for the choice of catalyst in the actual liquid-phase hydrogenation system.
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CATALYSIS LETTERS
·
2021
·Vol. 152
·期 3
·669-678
·
IF 3.186
Niu Ling,Du Jianmei,Jiang Daochuan,Du Haiwei,Lin Xiangang,Xu Jiahui,Li Zhongjun,Zhu Chuhong,Gu Lina,Bi Hong,Yuan Yupeng
Carbon defects in graphitic carbon nitride (g-CN) can modulate the electronic structure for efficient separation of electron–hole pairs, and thereby potentially enhance the photocatalytic H 2 generation. However, the mechanism on the separation of electrons and holes in C defect-modified g-CN still remains unclear. Here we report an autogenic ammonia gas route via in-situ urea decomposition to create carbon defects in g-CN for realizing increased photocatalytic H 2 generation rate of 36.62 µmol h −1 under visible light exposure, which is 10 times higher than that of g-CN obtained in the absence of autogenic ammonia gas (~ 3.63 µmol h −1 ). Illustrated by the density functional theory calculations, the C defects can not only reduce the band gap for increased light harvesting, but also delocalize the π electrons in valence band (VB) and conduction band (CB) for efficient charge transfer. Such delocalization of π electrons facilitates the efficient separation of electrons in LUMO and holes in HOMO, then promoting the photocatalytic H 2 generation. Therefore, the creation of C defects can be used as an effective route to delocalize the π electrons in g-CN for efficient photocatalytic H 2 generation. Graphical Abstract
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Yu Qin,Li Xu,Liying Liu,Zhongwei Ding
An original synthesis strategy for tubular zeolitic imidazolate framework (ZIF) membranes was developed by the deposition of a novel porous amorphous hybrid material prepared by 3-isocyanatopropyltrimethoxysilane (IPTMS) and ZIF-8 crystals onto a coarse macroporous α-Al2O3 tubular support. This porous amorphous hybrid material (ZIF-8-IPTMS) not only strongly adhered to the support but also repaired the defects to make the support surface smooth due to the abundant hydroxyl groups and the appropriate particle size. Using this synthesis strategy, we successfully prepared a high-quality ZIF-8 membrane on an inorganic α-Al2O3 tubular support via the sufficient heterogeneous nucleation sites provided by the amino groups of ZIF-8-IPTMS. This ZIF-8 membrane with an ultrathin thickness of approximately 0.9 μm was prepared, and its ideal H2/CO2 selectivity increased as the temperature increased. The membrane exhibited a competitive selectivity of 13.8 with a remarkably high H2 permeance of 1.46 × 10–5 mol·m–2·s–1·Pa–1 at 90 °C and 0.1 MPa. H2/CO2 binary gas permeation measurements indicated a separation factor of 9.2, and the H2 permeance was maintained at 0.83 × 10–5 mol·m–2·s–1·Pa–1 at 90 °C and 0.1 MPa. This synthesis strategy was also suitable to fabricate ZIF-67 membranes. The ZIF-67 membrane with a thickness of approximately 1.2 μm exhibited a H2/CO2 ideal selectivity of 5.3 and maintained a high H2 permeance of 1.06 × 10–5 mol·m–2·s–1·Pa–1 at 35 °C and 0.1 MPa.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
·
IF 5.816
Jun-Shuai Zhang,Wen-Chen Zhou,Wei-De Zhang,Yu-Xiang Yu
Developing earth abundant, active and stable photocatalysts for water splitting is a critical but challenging procedure for efficient conversion and storage of sustainable energy. Here, a ternary photocatalyst was rationally prepared for efficient H 2 production by covalently anchoring a nickel molecule cocatalyst (NiL) onto graphitic carbon nitride nanosheets (CN) and introducing nickel oxides (NiO x ) as hole-transport materials. The lower H 2 overpotential by NiL and the faster separation of photoinduced carriers by NiO x nanoparticles account for the efficient H 2 generation of CN without the help of noble metals. Eventually, the prepared NiL/NiO x /CN catalyst exhibited excellent performance for H 2 evolution (289 μmol g −1 h −1 ) in TEOA solution under visible light irradiation , which is superior to 3NiL/CN (161 μmol g −1 h −1 ) and CN (Null). Furthermore, a possible mechanism of photocatalytic H 2 production for NiL/NiO x /CN is proposed based on a series of electrochemical measurements. The noble-metal-free photocatalyst developed in this work will pave a new way to synthesize low-cost multicomponent photocatalysts for solar conversion.
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NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 45
·期 1
·217-222
·
IF 3.288
Chao Zhang,Xi Cheng,Baoquan Liu,Zhenmei Guo,Guangxiang He,Zhiguo Lv
Hexagonal wurtzite CdS has been regarded as one of the most promising semiconductors for photocatalysis. However, its water splitting performance under visible-light irradiation is seriously limited due to the high charge carrier recombination. In order to solve this limitation, we facilely prepared 2D hexagonal wurtzite CdS nanoplates (HWCs) with exposed (110) and (112) crystal facets via a water bath strategy. The visible-light responsivity of the HWCs exhibited an obvious red shift and, accordingly, the band gap was narrowed from 2.31 to 2.12 eV. Besides, the HWCs showed an excellent visible-light H2 evolution rate of ca. 6214.5 μmol h−1 g−1 without cocatalysts due to the enhanced charge carrier separation between the (110) and (112) crystal facets. Finally, a possible photocatalytic mechanism for HWCs was tentatively proposed. This work will be beneficial for designing and fabricating powerful mono-component photocatalysts.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Taotao Ji,Yanwei Sun,Yi Liu,Mingrun Li,Fei Wang,Liangliang Liu,Gaohong He,Yi Liu
Layered molecular sieve membranes containing uniform interlayer galleries have offered unprecedented opportunities to reach a performance far beyond the Robeson upper bound line. In this study, we took the initiative to prepare layered zirconium phenylphosphonate (ZrPP) molecular sieve membranes with optimized microstructure on tetragonal zirconia (t-ZrO2) buffer layer-modified porous α-Al2O3 substrates by facile in situ hydrothermal growth. Relying on the 3.2 Å-sized gallery height and preferential CO2 adsorption behavior, prepared ZrPP membranes showed exceptional H2/CO2 selectivity (>100) as well as considerable H2 permeability. Furthermore, extraordinary thermal, mechanical, and chemical stability of ZrPP membranes made them potentially attractive for long-term operations under harsh conditions.
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Journal of Energy Chemistry
·
2020
·
IF 7.216
Zhanghui Xie,Shan Yu,Xiang-Bing Fan,Shiqian Wei,Limei Yu,Yunqian Zhong,Xue-Wang Gao,Fan Wu,Ying Zhou
Photocatalytic splitting of hydrogen sulfide (H 2 S) for hydrogen evolution is a promising method to solve the energy and environmental issues. In this work, S,N-codoped carbon dots (S,N-CDs)/graphitic carbon nitride (g-C 3 N 4 ) nanosheet is synthesized by hydrothermal method as an efficient photocatalyst for the decomposition of H 2 S. In addition to the characterization of the morphology and structure, chemical state, optical and electrochemical performances of S,N-CDs/g-C 3 N 4 , hydrogen evolution tests show that the activity of g-C 3 N 4 is improved by introducing S,N-CDs, and the enhancement depends strongly on the wavelength of incident light. The photocatalytic hydrogen production rate of S,N-CDs/g-C 3 N 4 composite reaches 832 μmol g −1 h −1 , which is 38 times to that of g-C 3 N 4 under irradiation at 460 nm. Density functional theory calculations and electron paramagnetic resonance as well as photoluminescence technologies have altogether authenticated that the unique wavelength-dependent photosensitization of S,N-CDs on g-C 3 N 4 ; meanwhile, a good match between the energy level of S,N-CDs and g-C 3 N 4 is pivotal for the effective photocatalytic activity. Our work has unveiled the detailed mechanism of the photocatalytic activity enhancement in S,N-CDs/g-C 3 N 4 composite and showed its potential in photocatalytic splitting of H 2 S for hydrogen evolution.
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APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Sheng Zhao,Jing Xu,Min Mao,Lingjiao Li,Xuanhao Li
Based on hollow spherical NiCo 2 S 4 , Zn x Cd 1-x S with adjustable band structure was used to construct a composite for photocatalytic hydrogen evolution. The hollow spherical structure of NiCo 2 S 4 gives Zn x Cd 1-x S more contact positions to form a stable heterojunction. Through the band structure adjustment for Zn x Cd 1-x S, the induced electron transfer model was transformed into Z-scheme, which effectively enhances the photo-produced carrier separation efficiency of the composite material. At the same time, the fast electron transfer is realized by the great conductivity of the hollow spherical NiCo 2 S 4. This allows the composite material to obtain a shorter average lifetime of PL (0.15 ns) compared to Zn 0.5 Cd 0.5 S (3.9 ns). The composite NiCo 2 S 4 @Zn 0.5 Cd 0.5 S with Z-scheme heterojunction exhibited excellent photocatalytic HER activity and stability due to its unique spatial structure and efficient Z-scheme electron transfer path. The optimized composite NiCo 2 S 4 @Zn 0.5 Cd 0.5 S 1:1 photocatalytic HER rate reached 233.68 μmol . h −1 , which is equivalent to 5.81 times that of Zn 0.5 Cd 0.5 S (40.25 μmol . h −1 ).
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
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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