CHINESE JOURNAL OF CATALYSIS
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2023
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IF 16.5
Defa Liu,Bin Sun,Shuojie Bai,Tingting Gao,Guowei Zhou
Solar-powered semiconductor photocatalysis is considered a powerful strategy for addressing environmental pollution and energy crisis. Nevertheless, the separation and transfer abilities of photogenerated photocatalysts remain unsatisfactory. Herein, dual Ti 3 C 2 nanosheets/Ag co-catalysts synergistically decorated hierarchical flower-like TiO 2 microspheres for boosting photocatalytic H 2 production were fabricated by electrostatic self-assembly and subsequent photoreduction procedures. The optimal Ag/Ti 3 C 2 /TiO 2 composite demonstrated an excellent photocatalytic H 2 -production rate of 1024.72 μmol g −1 h −1 under simulated solar irradiation, achieving nearly 40, 2.3, and 1.8 folds with respect to that obtained on pristine TiO 2 , optimized Ti 3 C 2 /TiO 2 composite, and Ag/TiO 2 composite, respectively. The considerably improved photocatalytic H 2 -production activity is associated with the synergistic effect of the hierarchical flower-like structure of TiO 2 , excellent electrical conductivity of Ti 3 C 2 , and surface plasmon resonance effect of Ag, which enhances the light absorption capacity and promotes the separation and transfer of photogenerated carriers. This study provides insight into the design of high-efficiency photocatalysts with dual co-catalysts for solar H 2 production.
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Energy & Environmental Materials
·
2023
·
IF 15
Fan Liu,Xinghong Cai,Yang Tang,Wenqian Liu,Qianwei Chen,Peixin Dong,Maowen Xu,Yangyang Tan,Shujuan Bao
Electrocatalytic hydrogen evolution and sulfion (S 2− ) recycling are promising strategies for boosting H 2 production and removing environmental pollutants. Here, a nano-Ni-functionalized molybdenum disulfide (MoS 2 ) nanosheet was assembled on steel mesh (Ni-MoS 2 /SM) for use in sulfide oxidation reaction-assisted, energy-saving H 2 production. Experimental and theoretical calculation results revealed that anchoring nano-Ni on high-surface-area slack MoS 2 nanosheets not only optimized catalyst adsorption of polysulfides but also played an important role in promoting hydrogen evolution reaction kinetics by absorbing OH ad , thereby greatly enhancing the catalytic performance toward sulfide oxidation reaction and hydrogen evolution reaction. Meanwhile, the Ni/MoS 2 -based hydrogen evolution reaction + sulfide oxidation reaction system achieved nearly 100% hydrogen production efficiency and only consumed 61% less power per kWh than the oxygen evolution reaction + hydrogen evolution reaction system, which suggested our proposed Ni-MoS 2 and novel hydrogen production system are promising for sustainable energy production.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
·
IF 7.2
Fang He,Hong Zhong,Meng Wang,Hubo Yuan,Zhenxing Wang,Shaoqin Peng,Yuexiang Li
All carbon-based CG/M − CN rectangular nanotubes have been constructed by a facile molten salt thermal condensation of melamine and glucose. In the molten salt fluid, the glucose is carbonized into graphene-like (CG) nanosheets acting as an electron acceptor , and the melamine thermally condenses into carbon nitride (M − CN) rectangular nanotube acting as an electron donor . The 0.5 wt% CG/M − CN nanotubes display a photocatalytic H 2 evolution rate of 2345 μmol h −1 g −1 , which is 1.52 times higher than that of M-CN. Moreover, without loading Pt co-catalyst, the 0.5 wt% CG/M − CN nanotubes show a 12.75 times higher photocatalytic H 2 evolution rate than that of M-CN. It is revealed that the graphene-like CG nanosheets not only can act as an electron acceptor boosting charge carrier separation, but also function as a HER cocatalyst for M-CN. Our work provides a new insight for the development of all carbon-based photocatalysts for energy-related applications.
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Molecular Catalysis
·
2023
·
IF 4.6
Fukun Li,Ronghe Yang,Ziting Du,Jinhang Dai,Xingmin Wang,Ning Li,Xianming Zhang,Yunqi Liu,Haifeng Gong,Zhenping Cai,Junjun Shi
Biochemicals and biofuel derived from biomass conversion have received much attention over past decades. Alkyl levulinates are considered as promising building block chemicals and green fuel additive. This work presents a facile and efficient catalytic strategy for one pot cascade conversion of furfural to alkyl levulinates over rare earth metal trifluoromethanesulfonates (RE(OTf) 3 ) in alcohol without external H 2 . Experimental results demonstrate that RE(OTf) 3 binds to the alcohol ((OTf) 3 -RE-O(H)R), possessing both Brønsted acid and Lewis acid, plays a key role for this cascade process. Meanwhile, the selectivity of alkyl levulinate is closely related to charge density of selected metal ion and the reduction potential of the selected alcohol. Among various tests, Lu(OTf) 3 , possessing the greatest charge density, exhibits the best catalytic activity in the lowest reduction potential of 2-propanol. 100% furfural conversion and 52.8% ispropanyl levulinate yield can be achieved at 190°C within 45 min. This catalyst can be recycled five times by direct vacuum distillation and regenerated by oxidative elimination of formed humins. Besides, a plausible reaction mechanism is also proposed.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Xiaohang Yang,Weilun Yu,Wensi Wang,Da Wang,Qiyao Wang,Xuyang Huo
A strategy of tuning the size of In 2 O 3 nanocube was employed to change the surface property of g–C 3 N 4 –In 2 O 3 heterojunction to boost its photocatalytic H 2 production. In the type II g–C 3 N 4 –In 2 O 3 heterojunction, the change on the size of In 2 O 3 nanocube (30, 60 and 120 nm) could regulate visible light utilization ability and photoelectric conversion efficiency of photogenerated charge carriers. The directional transfer of charge carriers caused the accumulation of photoexcited electron in plasmonic In 2 O 3 and localized electric field enhancement. The intensity and spatial distribution of localized electric field could be tuned by the adjustable size of In 2 O 3 nanocube. Therefore, the obtained g–C 3 N 4 –In 2 O 3 heterojunction with an optimal size of In 2 O 3 nanocube (60 nm) exhibited supreme photocatalytic H 2 evolution rate of 3.1 mmol h −1 g −1 with a high apparent quantum efficiency of 5.27%, which was 7.5 times higher than that of bare g-C 3 N 4 nanosheet (0.4 mmol h −1 g −1 ).
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Fang He,Hubo Yuan,Huayan You,Zhenxing Wang,Shaoqin Peng,Yuexiang Li
Building carbon nitride (CN)-based core shell heterostructures is an effective strategy to enhance the photocatalytic performance and stability by optimize the interface area and protect the CN core, respectively. Moreover, by fabricating the porous structures in core shells can further optimize the light absorption, charge separation, and mass transfer. Herein, we have constructed porous C-PDA–CN–ms core-shell heterostructures through a facile green molten salt (ms) sculpture the polydopamine (PDA) derived carbon (C-PDA) shells with CN core. In which, the C-PDA-CN core-shells arise from in situ polymerization of dopamine (DA) on the surface of melamine to form PDA@melamine coatings followed by thermal polycondensation . The molten salts at high-temperature act as a green fluid immersing in and out of C-PDA-CN core-shells to further produce porous structures. The 1 wt% C-PDA–CN–ms with porous core-shell structures display photocatalytic H 2 evolution rate of 3830 μmol h −1 g −1 , which is 20.8 times enhancement of 1 wt% C-PDA-CN core-shells, even 73.6 times higher than that of pristine CN. It reveals that the porous and core-shell heterostructures endow C-PDA–CN–ms enhanced light absorption, various charge transport channels for improved charge carrier separation and transfer, contributing to the superior photocatalytic H 2 evolution performance. Our work opens a new window for the green construction of porous core-shell heterostructures of CN-based photocatalysts .
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Tao Yan,Jianhua Yang,Jinming Lu,Liang Zhou,Yan Zhang,Gaohong He
Recently, pillar-layered MOF materials have attracted much attention and shown great potential in separation application due to their fine pore size/channel and pore surface chemistry tunability and designability. In this work, we reported an effective and universal synthesis strategy for preparing ultra-microporous Ni-based pillar-layered MOF [Ni2(L-asp)2(bpy)] (Ni-LAB) and [Ni2(L-asp)2(pz)] (Ni-LAP) (L-asp = L-aspartic acid, bpy = 4,4′-bipyridine, pz = pyrazine) membranes on a porous α-Al2O3 substrate with high performance and good stability by secondary growth. Through this strategy, the seed size reduction and screening engineering (SRSE) is proposed to obtain uniform sub-micron size MOF seeds by high-energy ball milling-combined solvent deposition. This strategy not only effectively addresses the issue of obtaining the uniform small seeds being significant for secondary growth but also provides an approach for the preparation of Ni-based pillar-layered MOF membranes where the freedom of synthesizing small crystals is lacking. Based on reticular chemistry, the pore size of Ni-LAB was narrowed by making use of shorter pillar ligands of pz instead of the longer pillar ligand of bpy. The prepared ultra-microporous Ni-LAP membranes exhibited a high H2/CO2 separation factor of 40.4 with H2 permeance of 9.69 × 10–8 mol m–2 s–1 Pa–1 under ambient conditions and good mechanical and thermal stability. The superiority of the tunable pore structure and the remarkable stability of these MOF materials showed great potential for industrial H2 purification. More importantly, our synthesis strategy demonstrated the generality for preparation of MOF membranes, enabling the regulation of membrane pore size and surface functional groups by reticular chemistry.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Yixuan Lv,Dandan Ma,Chao Yang,Kunli Song,Le Shi,Yonghong Cheng,Chunming Niu,Jian-Wen Shi
Lead-free halide perovskites have enormous superiority in photoelectric devices, but low photocatalytic hydrogen evolution (PHE) hinders their application in photocatalysis. Here, a heterojunction composed of CsCu 2 I 3 (CCI) perovskite and graphite carbon nitride (CN) is constructed by in-situ hot-injection method for the first time. The resultant CCI/CN presents a significantly enhanced PHE performance from hydroiodic acid (HI) splitting with a PHE rate of 2212 umol/g/h, which is four times higher than CCI and nearly ten times higher than CN. It is revealed that a unique N-I bond is formed by the connection of N in CN and I in CCI at the interface between CN and CCI, which serves as a fast channel for the transfer of photogenerated electrons to establish a type II mechanism, effectively promoting the PHE performance. This study provides ideas and methods for the construction of type II photocatalyst for hydrogen production using lead-free halide perovskite.
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RSC Advances
·
2023
·Vol. 13
·期 13
·8915-8922
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IF 3.9
Tong Zhou,Haitang Wei,Bin Xiao,Tianping Lv,Liangfei Duan,Qingjie Lu,Jin Zhang,Yumin Zhang,Qingju Liu
One of the most promising strategies for producing hydrogen is photocatalytic water splitting, in which the photocatalyst is a key component. Among many semiconductor photocatalysts, g-C3N4 has attracted great attention due to its narrow band gap, excellent stability and low cost. However, practical application is limited by its poor intrinsic activity. In this work, a high-performance porous g-C3N4 (PCN) photocatalyst with anchored Cu single atoms (CuSAs) was synthesized by a one-step co-heating approach. The obtained Cu1.5–PCN displays an excellent hydrogen evolution rate (HER) of 2142.4 μmol h−1 g−1 under visible light (=420 nm), which is around 15 and 109 times higher than those of PCN and bulk g-C3N4, respectively. In addition, it also shows good stability during H2 evolution. The results of experimental research and DFT simulations indicate that the single Cu ions formed bonds with the N-ring and these remain stable. Meanwhile, the special electronic structure of the Cu–N charge bridge extends the light absorption band to the visible-light region (380–700 nm). This high-performance and low-cost photocatalyst has great potential in solar energy conversion.
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Journal of Experimental Nanoscience
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2022
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IF 2.024
Zhen-Hong He,Yuan-Yuan Wei,Na Li,Yong-Chang Sun,Shao-Yan Yang,Kuan Wang,Weitao Wang,Xiaoxue Ma,Zhao-Tie Liu
Chemical utilization of CO2 is one of the fundamental strategies to synthesize value-added chemicals and reduce the CO2 emission. N-formyl-1,2,3,4-tetrahydroisoquinoline derivatives (FTHIQs) are important chemicals for the synthesis of medical intermediates and alkaloids. N-formylation of isoquinoline derivatives (IQs) with CO2 is an ideal protocol to synthesize the FTHIQs and utilize the CO2 source. In the present work, we prepared a heterogeneous Ru/ZIF-8 catalyst with a Ru loading of 2 wt% by a simple impregnation method and assessed its performances in the N-formylation of IQs and CO2 with H2. The Ru/ZIF-8 catalyst offered high IQ conversion of 98% and FTHIQ selectivity of 93% in the reaction under relatively mild conditions (150 °C, 2 MPa CO2, and 6 MPa H2). The catalyst possessed good universality and reusability, showing a potential in wide application of N-formylation of highly unsaturated nitrogen-containing isoquinolines.
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ACS Applied Materials & Interfaces
·
2018
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IF 8.097
Fangfang Yang,Mian Wu,Yuchao Wang,Saeed Ashtiani,Heqing Jiang
Metal–organic framework (MOF) nanosheets have emerged as promising materials for the construction of molecular sieve membranes due to their nanoscale thickness and highly oriented pore arrays. However, the development of defect-free MOF nanosheet membranes from rigid MOF nanosheets with efficient permselectivity and robust mechanical strength still remains a big challenge. Herein, we develop a facile GO-induced assembly strategy to design continuous and uniform two-dimensional MOF composite membranes, in which the copper 1,4-benzene dicarboxylate (CuBDC) nanosheets present a layer-stacking arrangement. With the assistance of flexible GO, the voids between the junctions of rigid MOF nanosheets are well-repaired, and the interlayer bonding interactions are strengthened, resulting in the fabrication of a continuous nanosheet membrane with robust mechanical strength. The obtained MOF nanosheet-based membranes display remarkable H2/CO2 separation performance with a superior H2 permeance of 9.6 × 10–7 mol m–2 s–1 Pa–1 and an ideal separation selectivity of 95.1 due to the well-defined size exclusion effect, showing great promise for H2 separation and purification. The repair strategy described here could also provide the blueprint for the development of other nanosheet-based membranes.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2018
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IF 4.229
Meiqing Chen,Pingxiao Wu,Yajie Zhu,Shanshan Yang,Yonghong Lu,Zhang Lin
In order to enhance the visible light-driven photocatalytic H 2 production activity of CdZnS, an ethylenediamine-assisted hydrothermal pathway was used to synthesize CdxZn1-xS(en) with different Cd/Zn molar ratios . It was found out that the prepared Cd 0.5 Zn 0.5 S(en) possessed the highest photocatalytic H 2 production rate of 13539.0 μmol h −1 g −1 that was higher than that of CdZnS. The key to this achievement could be ascribed to the stacking faults formation, the optimum band gap with conduction band position and small crystallite size. Based on this, Cd 0.5 Zn 0.5 S(en) was modified by NiS for further improving the activity. The obtained Cd 0.5 Zn 0.5 S(en) NiS with NiS loading content of 0.25 wt% exhibited much higher photocatalytic H 2 production rate, reaching up to 38187.7 μmol h −1 g −1 that were among the highest efficiencies for semiconductor photocatalysts ever reported. It was confirmed that the nanosized NiS anchored on Cd 0.5 Zn 0.5 S(en) interface, acting as electron trapping sites, attributed to the spatial suppressions of electron-hole recombination. Meanwhile, the NiS loaded on the surface optimized the photogenerated electron transfer pathway between the semiconductor materials that gives rise to significantly enhanced photocatalytic activity . This study would put forward a facile method for developing high photocatalytic activity and low-cost catalytic material for H 2 production, which provide a new thought to address the global energy crisis and the environmental contamination.
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