JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Guang Yang,Hao Zhang,Mingyu Dou,Hua Yang,Xingliang Yin,Dacheng Li,Haitao Zhao,Jianmin Dou
To enhance the photocatalytic activity, loading proper semiconductor with high efficiency and low cost is one of the most valid approaches. Herein, various amounts of CoWO 4 as a novel metal-free material were loaded on Mn 0.47 Cd 0.53 S (MCS) nanorods for photocatalytic hydrogen production reaction. The CoWO 4 /Mn 0.47 Cd 0.53 S-25 (CW/MCS-25) exhibits the highest hydrogen production rate of 41.53 mmol·h −1 ·g −1 in the Na 2 S/Na 2 SO 3 system, which is about 2.68 times higher than that of pristine MCS. The Mapping and HRTEM reveals the deposited of CoWO 4 on the MCS. The detailed analyses of XPS, EIS, TRPL spectra and transient photocurrent responses indicate that CoWO 4 and MCS interacted closely and the photogenerated electrons of CoWO 4 can be transferred into MCS. In particular, the introduction of CoWO 4 can further transfer the photogenerated holes of MCS, thereby inhibiting the photocorrosion of MCS and improving photocatalytic activity. This work provides a reference for the exploration of noble metal-free composite material and shows great potential in the photocatalytic application.
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ACS Applied Energy Materials
·
2021
·
IF 6.024
Dewei Yao,Hongmei Yu,Wei Song,Xueqiang Gao,Xinye Sun,Guang Jiang,Jinkai Hao,Zhigang Shao
To reduce cost and energy consumption of fuel cell vehicles, constructing membrane electrode assemblies (MEAs) with low Pt loading and outstanding performance at low relative humidity (RH) conditions is reported. A catalyst layer based on porous Pt–Ni nanobelt arrays was prepared, in which the strained catalyst enhanced the catalytic activity and the oriented nanobelt array structure provided convenient mass transport channels. The porous Pt–Ni nanobelt arrays were prepared by the magnetron sputtering of Pt and Ni on a sacrificed template and then washed with acid. Consequently, the catalyst layer based on the porous Pt–Ni nanobelt arrays exhibited superior fuel cell performance in H2/air conditions and RH 40%. The performance of the MEA with porous Pt–Ni nanobelt arrays reach 366.6 and 597.6 mW cm–2 with Pt loadings of 36.5 μg cm–2/36.5 μg cm–2 and 108.9 μg cm–2/108.9 μg cm–2 at the cathode/anode, respectively. A conventional CCM with the Pt loading of 100 μg cm–2/200 μg cm–2 at the cathode/anode served as the benchmark, and the cell performance was 230.5 mW cm–2. Apart from that, the Pt nanobelt arrays without a porous structure (100.8 g cmPt–2/100.8 μg cmPt–2) serving as another benchmark achieved a performance of 504.7 mW cm–2. The superior performance of the porous Pt–Ni nanobelt arrays is attributed to the convenient mass transport pathway and the high activity of the porous Pt–Ni nanobelt.
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Solar RRL
·
2021
·Vol. 5
·期 11
·2100536
·
IF 8.582
Yujie Liu,Qiaohong Zhu,Muhammad Tayyab,Liang Zhou,Juying Lei,Jinlong Zhang
Semiconductor supported noble metal nanoparticles are widely used in H 2 evolution. Due to the high cost and low catalytic efficiency of noble metals, single-atom catalysts (SACs) are considered as very potential materials to overcome these shortcomings. Herein, the construction of the ZnO–ZnS heterojunction with an excess amount of Zn vacancies promotes the separation of charge carriers and improves the utilization of electrons. Meanwhile, the zinc vacancies on ZnS provide effective anchor sites for Pt atoms, which is beneficial to obtain highly dispersed single Pt atoms catalyst (ZOS-SAPt). Due to the formation of an intermediate energy level by zinc vacancies, the introduction of Pt single atoms promotes the novel type-V electron transport from the conduction band of ZnO to the intermediate energy level and then to the Pt atom. The type-V electron transport not only retains the high reduction potential of photogenerated electrons, but also avoids the loss of carriers. The resultant ZOS-SAPt shows outstanding photocatalytic performance for H 2 evolution under simulated sunlight, reaching 9.6 mmol g −1 h −1 , which is 201 times that of ZnO–ZnS. These results provide important information for further development of photocatalysts.
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NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 47
·22123-22132
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IF 3.591
Jing Liu,Dianming Li,Xiaofeng Liu,Jie Zhou,Hong Zhao,Nü Wang,Zhimin Cui,Jie Bai,Yong Zhao
Hydrogen evolution and dye degradation catalyzed by environmentally benign and inexpensive photocatalyst in aqueous solution is regarded as a promising avenue to effectively address the global energy and environmental crisis. It is difficult for traditional photocatalysts to perform efficient light harvesting, with conducive recycling and promoted charge separation and transport, which limit practical applications in photocatalytic conversion. In this study, a facile template-assisted coaxial electrospinning approach was explored to successfully build close contacted heterojunctions within the interface of g-C3N4 nanosheets and hollow porous TiO2 nanofibers, which significantly increased the separation efficiency of photo-induced electron–hole pairs in the visible-light region. A hollow and porous structure with abundant surface-active sites assisted in inducing multiple light reflection for more efficient light harvesting. Moreover, one dimensional TiO2/g-C3N4 composite nanofibers with a large length-to-diameter ratio would be more attractive for recovery. At the optimal g-C3N4 loading, hollow porous TiO2/g-C3N4-50% nanofibers exhibited the highest rate of hydrogen evolution and RhB degradation. The enhanced photocatalytic performance of hollow porous TiO2/g-C3N4 composite photocatalysts was mainly attributed to the synergistic effect of the hollow porous architecture and heterojunction. This work might make a significant contribution to insight into preparing hollow structure heterogenous nanofiber photocatalysts with improved activities in hydrogen generation and pollutant degradation.
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ADVANCED MATERIALS
·
2021
·Vol. 33
·期 39
·2101455
·
IF 30.849
Yangsen Xu,Mingjian Fan,Wenjuan Yang,Yonghao Xiao,Lingting Zeng,Xiao Wu,Qinghua Xu,Chenliang Su,Qianjun He
The efficient utilization of near-infrared (NIR) light for photocatalytic hydrogen generation is vitally important to both solar hydrogen energy and hydrogen medicine, but remains a challenge at present, owing to the strict requirement of the semiconductor for high NIR responsiveness, narrow bandgap, and suitable redox potentials. Here, an NIR-active carbon/potassium-doped red polymeric carbon nitride (RPCN) is achieved for by using a similar-structure dopant as the melamine (C 3 H 6 N 6 ) precursor with the solid KCl. The homogeneous and high incorporation of carbon and potassium remarkably narrows the bandgap of carbon nitride (1.7 eV) and endows RPCN with a high NIR-photocatalytic activity for H 2 evolution from water at the rate of 140 µmol h −1 g −1 under NIR irradiation (700 nm ≤ λ ≤ 780 nm), and the apparent quantum efficiency is high as 0.84% at 700 ± 10 nm (and 13% at 500 ± 10 nm). A proof-of-concept experiment on a tumor-bearing mouse model verifies RPCN as being capable of intratumoral NIR-photocatalytic hydrogen generation and simultaneous glutathione deprivation for safe and high-efficacy drug-free cancer therapy. The results shed light on designing efficient photocatalysts to capture the full spectrum of solar energy, and also pioneer a new pathway to develop NIR photocatalysts for hydrogen therapy of major diseases.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jingwen Zhang,Chuchu Cheng,FangShu Xing,Cheng Chen,Caijin Huang
Engineering semiconductor materials with vacancies and co-catalysts is a valid method to improve their photocatalytic performance. Herein, we prepared S vacancies-rich Mn 0.3 Cd 0.7 S nanorods modified with β-Ni(OH) 2 nanoparticles through solvothermal and co-precipitation strategies. The as-obtained 0D/1D β-Ni(OH) 2 /Mn 0.3 Cd 0.7 S nanorods exhibit excellent visible-light H 2 -production activity up to 71.09 mmol g −1 h −1 , 5.23 times higher than pure Mn 0.3 Cd 0.7 S and better than 1 wt% Pt/Mn 0.3 Cd 0.7 S and most reported Mn x Cd 1−x S-based catalysts. The apparent quantum yield reaches 46.68% at λ = 420 nm. We found that the presence of S vacancies and β-Ni(OH) 2 enhances the transfer/separation of photogenerated carriers and increases reaction sites, which is beneficial to photocatalytic H 2 -production reaction. This work proposes a new idea for the application of metal hydroxide co-catalysts and S vacancies in sulfide materials for photocatalytic H 2 production.
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DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 27
·9529-9539
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IF 4.39
Xin Guo,Lina Kong,Jianping Xu,Jing Chen,Lan Li
Surface decoration of noble-metal cocatalysts on graphitic phase carbon nitride (g-C3N4) with high efficiency and trace content for water splitting is exciting but difficult to achieve. Herein, we report the anchoring of Au and metallic/oxidized Pt nanoparticles (NPs) on g-C3N4 as cocatalysts via a photoreduction process for enhancing photocatalytic H2 production. Au NPs are preferentially decorated on g-C3N4, which can control the formation of metallic/oxidized Pt complex species. The well dispersed Au and metallic/oxidized Pt NPs improved the light-harvesting and the photo-generated carrier separation of g-C3N4. G-C3N4 sequentially decorated with Au (0.3 wt%) and metallic/oxidized Pt (0.3 wt%) cocatalysts, exhibited the highest and stable H2 evolution rates of 2560 and 139 μmol h−1 g−1 under simulated sunlight and visible light (λ ≥ 420 nm) irradiation, respectively, compared to the samples that are simultaneously and sequentially decorated with the same content of Pt and Au on g-C3N4. The enhanced photocatalytic activity is attributed to the synergistic effect of Au and metallic/oxidized Pt cocatalysts, i.e., the effective localized surface plasma resonance coupling between Pt and Au NPs, as well as electron-sink function of metallic Pt, which promote the generation and transfer of more carriers from g-C3N4 to the Pt species, in addition to the superior hydrogen evolution capacity of metallic and oxidized Pt. This work maximizes the performance of noble-metal cocatalysts with minimized content and provides the possibility of realizing efficient solar-to-fuel conversion.
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Inorganic Chemistry Frontiers
·
2020
·Vol. 8
·期 5
·1154-1165
·
IF 5.958
Kunqiao Li,Wanbao Wu,Yanqiu Jiang,Zhe Wang,Xing Liu,Junzhuo Li,Debin Xia,Xianzhu Xu,Jizhuang Fan,Kaifeng Lin
The Z-scheme photocatalytic system has great potential in solar energy conservation with simultaneous wide light-absorption range, efficient electron–hole pair separation and strong redox ability. Herein, a direct Z-scheme g-C3N4/MoO3 photocatalytic composite with oxygen vacancies is successfully fabricated via a facile in situ method of a one-pot pyrolysis strategy. The as-prepared g-C3N4/MoO3 possesses a porous architecture with increased specific surface area. The existence of an oxygen vacancy in MoO3 is verified by XPS, UV-DRS analysis and electrochemical measurements. The g-C3N4/MoO3 exhibits superior visible-light photocatalytic performance for water splitting, as evidenced by an about 17-fold (20.52 μmol h−1) increase in the rate of H2 evolution relative to pristine C3N4 (1.23 μmol h−1). According to the characterization results and boosted photocatalytic performance, the migration and separation of photoinduced charge carriers in g-C3N4/MoO3 follows a possible mechanism based on a Z-scheme photocatalytic system constructed by the oxygen vacancies. The O-vacancy functions as the recombination and storage center for fast charge transfer through two components. The combined effect of defective MoO3 and a Z-scheme interfacial heterojunction has achieved greatly enhanced photocatalytic performance. This work demonstrates the facilitation effect of an effective Z-scheme system involving oxygen vacancies on the charge transfer to enhance the photocatalytic activity for water splitting.
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CARBON
·
2020
·
IF 8.821
Jinqiao Li,Xiaoteng Liu,Huinan Che,Chunbo Liu,Chunxiang Li
Realizing the efficient utilization of photogenerated carriers is a pivotal process to access the efficient transformation of light energy . Herein, we firstly practice a facile template method to synthesize O-doped crystalline/none-crystalline g-C 3 N 4 embedded nano-homojunction photocatalysts (CMCCN-x). This nano-homojunction makes the crystalline phase sufficiently contact with amorphous phase and further facilitates the photoinduced electron transformation. Therefore, the best performance catalyst CMCCN-5 well integrates the advantages of crystal g-C 3 N 4 and amorphous g-C 3 N 4 , which exhibits an excellent photogenerated carrier separation ability and abundant photocatalytic hydrogen evolution reaction activity sites. Excellent performance in the separation and use of photogenic carriers endows CMCCN-5 with efficient utilization of photogenerated carriers. Although there is a limited light absorption range (<460 nm), the photocatalytic hydrogen evolution rate of CMCCN-5 is up to 203.66 μmol h −1 under the visible light irradiation, about 86 times higher than pristine g-C 3 N 4 . The AQY numbers of CMCCN-5 at 420 nm and 450 nm are up to 26.9% and 14.0%, respectively. Thus, the significant effectiveness is forcefully proved for the facile construction of O-doped g-C 3 N 4 crystalline/none-crystalline nano-homojunction.
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FUEL
·
2020
·
IF 5.578
Muhammad Irfan,Aimin Li,Lei Zhang,Guozhao Ji,Yuan Gao
Catalytic gasification, coupled with in-situ CO 2 capture over Ni-CaO catalyst, is considered to be an effective approach for H 2 -rich and tar-free syngas production. However, the poor stability of Ni-CaO based catalyst raises a question regarding its large scale application. In this study, HfO 2 was used as a stabilizer and promoter for the Ni-CaO catalyst system. The stability of catalyst was evaluated through cyclic carbonation-calcination test with a thermogravimetric analyzer. The results showed that HfO 2 incorporated catalysts performed better stability towards cyclic CO 2 capture. The effect of different HfO 2 additions in catalyst, catalyst to municipal solid waste (C/MSW) ratio, gasification temperature, and moisture content (MC) of MSW was investigated on syngas composition, H 2 yield, dry gas yield (DGY) and product distribution (syngas, tar and char). The results indicated that H 2 yield was improved from 212 mL/g (without catalyst) to 442 mL/g with Ni-CaO (NC) catalyst and further improved with the application of HfO 2 promoted catalysts (Ni-CaO-HfO 2 ). The catalyst with 20% HfO 2 (NCH-20) exhibited maximum H 2 yield of 597 mL/g. Moreover, a significant reduction in tar content from 8.79 wt% (without catalyst), 3.19 wt% (with Ni-CaO) to 2.81 wt% (with NCH-20) was also recorded with HfO 2 promoted catalysts.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
·
IF 4.939
Xinwei Jiang,Qiang Liu,Chuchu Cheng,FangShu Xing,Cheng Chen,Caijin Huang
Developing a suitable and low-cost co-catalyst is highly desired for promoting photocatalytic water splitting of H 2 production. Herein, we adopted a simple in situ photodeposition strategy by coupling Mn 0.5 Cd 0.5 S with non-noble co-catalyst Ni 2 P to construct Ni 2 P/Mn 0.5 Cd 0.5 S composites and achieved obviously improved H 2 amount (31.83 mmol/h/g) in visible-light region, which is nearly 2.8 times than that of pure Mn 0.5 Cd 0.5 S. Such photocatalytic performance is in a relatively superior position among Mn x Cd 1−x S-based photocatalysts . The apparent quantum efficiency of Ni 2 P/Mn 0.5 Cd 0.5 S-7 composites reaches 32% at 420 nm. Through optical and photoelectrochemical measurements, a possible mechanism was proposed, it was found that the interface between metalloid Ni 2 P and Mn 0.5 Cd 0.5 S contacts closely, which facilitates transfer and separation of charge carriers, thus promotes the reduction of H + to H 2 . This study provides a new design of cut-price, high-efficiency photocatalyst for H 2 evolution.
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Nature Communications
·
2020
·Vol. 11
·期 1
·1-13
·
IF 12.121
Liu Yi,Zhang Jihua,Li Yapeng,Qian Qizhu,Li Ziyun,Zhu Yin,Zhang Genqiang
Replacing sluggish oxygen evolution reaction (OER) with hydrazine oxidation reaction (HzOR) to produce hydrogen has been considered as a more energy-efficient strategy than water splitting. However, the relatively high cell voltage in two-electrode system and the required external electric power hinder its scalable applications, especially in mobile devices. Herein, we report a bifunctional P, W co-doped Co 3 N nanowire array electrode with remarkable catalytic activity towards both HzOR (−55 mV at 10 mA cm −2 ) and hydrogen evolution reaction (HER, −41 mV at 10 mA cm −2 ). Inspiringly, a record low cell voltage of 28 mV is required to achieve 10 mA cm −2 in two-electrode system. DFT calculations decipher that the doping optimized H* adsorption/desorption and dehydrogenation kinetics could be the underlying mechanism. Importantly, a self-powered H 2 production system by integrating a direct hydrazine fuel cell with a hydrazine splitting electrolyzer can achieve a decent rate of 1.25 mmol h −1 at room temperature.
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