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Superior performance in visible-light-driven hydrogen evolution reaction of three-dimensionally orderedmacroporous SrTiO decorated with ZnCdS

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1561-1571 doi: 10.1007/s11705-021-2089-z

摘要： It is of broad interest to develop emerging photocatalysts with excellent light-harvesting capacity and high charge carrier separation efficiency for visible light photocatalytic hydrogen evolution reaction. However, achieving satisfying hydrogen evolution efficiency under noble metal-free conditions remains challenging. In this study, we demonstrate the fabrication of three-dimensionally ordered macroporous SrTiO3 decorated with ZnxCd1−xS nanoparticles for hydrogen production under visible light irradiation (λ>420 nm). Synergetic enhancement of photocatalytic activity is achieved by the slow photon effect and improved separation efficiency of photogenerated charge carriers. The obtained composites could afford very high hydrogen production efficiencies up to 19.67 mmol·g−1·h−1, with an apparent quantum efficiency of 35.9% at 420 nm, which is 4.2 and 23.9 times higher than those of pure Zn0.5Cd0.5S (4.67 mmol·g−1·h−1) and CdS (0.82 mmol·g−1·h−1), respectively. In particular, under Pt-free conditions, an attractive hydrogen production rate (3.23 mmol·g−1·h−1) was achieved, providing a low-cost and high-efficiency strategy to produce hydrogen from water splitting. Moreover, the composites showed excellent stability, and no obvious loss in activity was observed after five cycling tests.

关键词： three-dimensionally ordered macroporous SrTiO3     ZnxCd1–xS     visible light     hydrogen production     promotion mechanism    

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Fabrication of three-dimensional porous La-doped SrTiO3 microspheres with enhanced visible light catalytic

Dong Yang, Xiaoyan Zou, Yuanyuan Sun, Zhenwei Tong, Zhongyi Jiang

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 440-449 doi: 10.1007/s11705-018-1700-4

摘要：

In recent years, much effort has been focused on the development of the photocatalysts with high performance under visible light irradiation. In this paper, three-dimensional porous La-doped SrTiO3 (LST) microspheres were prepared by a modified sol–gel method, in which the agarose gel/SrCO3 microsphere and La2O3 were employed as the template and the La resource, respectively. The as-prepared LST microspheres exhibit a porous structure with a diameter of about 10 µm and a surface pore size of about 100 nm. The La element was doped into the crystal lattice of SrTiO3 by the substitution of La3+ for Sr2+. Therefore, the absorption edge of LST samples shifts toward the visible light region, and their photocatalytic activity for the Cr(VI) reduction is enhanced under visible light. Among all LST samples, LST-0.5 (the La3+ doping content is 0.5 wt-%) exhibited the highest visible-light photocatalytic activity, which can reduce 84% Cr(VI) within 100 min. This LST materials may become a promising photocatalyst for the facile treatment of wastewater containing poisonous heavy metal ions.

关键词： SrTiO3     La3+ doping     porous microsphere     visible-light photocatalysis     Cr(VI) reduction    

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Function-reversible facets enabling SrTiO nanocrystals for improved photocatalytic hydrogen evolution

《能源前沿（英文）》 doi: 10.1007/s11708-023-0894-4

摘要： It has been widely reported that, for faceted nanocrystals, the two adjacent facets with different band levels contribute to promoted charge separation, and provide active sites for photocatalytic reduction and oxidation reaction, respectively. In such cases, only one family of facets can be used for photocatalytic hydrogen evolution. Herein, by using SrTiO3 nanocrystals enclosed by {023} and {001} facets as a model photocatalyst, this paper proposed a strategy to achieve the full-facets-utilization of the nanocrystals for photocatalytic hydrogen via chemically depositing Pt nanoparticles on all facets. The photo-deposition experiment of CdS provided direct evidence to demonstrate that the {023} facets which were responsible for photooxidation reaction can be function-reversed for photocatalytic hydrogen evolution after depositing Pt nanoparticles, together with the {001} facets. Thus, the full-facets-utilization led to a much-improved activity for photocatalytic hydrogen, in contrast to those SrTiO3 nanocrystals with only {001} facets deposited by Pt nanoparticles via a photo-deposition method.

关键词： SrTiO3 nanocrystals     crystal facets     photocatalysis     hydrogen evolution    

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Enhanced photocatalytic water splitting with surface defective SrTiO

Junying LIU, Zhidong WEI, Wenfeng SHANGGUAN

《能源前沿（英文）》 2021年 第15卷 第1期   页码 700-709 doi: 10.1007/s11708-021-0735-2

摘要： Surface reconstructed SrTiO nanocrystals were synthesized by a thermal treatment process in presence of NaBH and SrTiO nanocrystals. The surface reconstruction of SrTiO nanocrystals is attributed to the introduction of surface oxygen vacancies or Ti sites (such as Ti and Ti ) during the hydrogenation treatment process. The light absorption and the charge transfer ability of SrTiO nanocrystals are simultaneously enhanced due to surface oxygen vacancies or Ti sites (such as Ti and Ti ), which are beneficial to photocatalytic water splitting. Meanwhile, these defects also change the redox potential of the photocatalysts. Since there existed a synergistic effect between the three, the ratio of hydrogen to oxygen production was also regulated.

关键词： SrTiO3     surface reconstruction     oxygen vacancies     photocatalytic water splitting    

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Real drive cycles analysis by ordered power methodology applied to fuel consumption, CO

Pol Masclans Abelló, Vicente Medina Iglesias, M. Antonia de los Santos López, Jesús Álvarez-Flórez

《环境科学与工程前沿（英文）》 2021年 第15卷 第1期 doi: 10.1007/s11783-020-1296-z

摘要： Abstract • New method named CAbOP is presented based on ordering data according to power. • Three emission models are used and their emission results compared. • Emissions data are analyzed in real driving cycles under CAbOP criteria. • Methodology to collect data and reconstruct lost data in real urban driving cycles. In this work three fuel consumption and exhaust emission models, ADVISOR, VT-MICRO and the European Environmental Agency Emission factors, have been used to obtain fuel consumption (FC) and exhaust emissions. These models have been used at micro-scale, using the two signal treatment methods presented. The manuscript presents: 1) a methodology to collect data in real urban driving cycles, 2) an estimation of FC and tailpipe emissions using some available models in literature, and 3) a novel analysis of the results based on delivered wheel power. The results include Fuel Consumption (FC), CO2, NOx and PM10 emissions, which are derived from the three simulators. In the first part of the paper we present a new procedure for incomplete drive cycle data treatment, which is necessary for real drive cycle acquisition in high density cities. Then the models are used to obtain second by second FC and exhaust emissions. Finally, a new methodology named Cycle Analysis by Ordered Power (CAbOP) is presented and used to compare the results. This method consists in the re-ordering of time dependant data, considering the wheel mechanical power domain instead of the standard time domain. This new strategy allows the 5 situations in drive cycles to be clearly visualized: hard breaking zone, slowdowns, idle or stop zone, sustained speed zone and acceleration zone. The complete methodology is applied in two real drive cycles surveyed in Barcelona (Spain) and the results are compared with a standardized WLTC urban cycle.

关键词： Cycle Analysis by Ordered Power (CAbOP)     Micro and macro models     Real drive cycle     NOx/PM10/CO2 emissions     Wheel mechanical power domain     Worldwide Harmonized Light-Duty Vehicles Test Cycle (WLTC)    

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Printability and hardening performance of three-dimensionally-printed geopolymer based on lunar regolith

《结构与土木工程前沿（英文）》 doi: 10.1007/s11709-023-0003-0

摘要： Using an in situ lunar regolith as a construction material in combination with 3D printing not only reduces the weight of materials carried from the Earth but also improves the automation of lunar infrastructure construction. This study aims to improve the printability of a geopolymer based on a BH-1 lunar regolith simulant, including the extrudability, open time, and buildability, by controlling the temperature and adding admixtures. Rheological parameters were used to represent printability with different water-to-binder ratios, printing temperatures, and contents of additives. The mechanical properties of the hardening geopolymer with different filling paths and loading directions were tested. The results show that heating the printed filaments with a water-to-binder ratio of 0.32 at 80 °C can adjust the printability without adding any additive, which can reduce the construction cost of lunar infrastructure. The printability of the BH-1 geopolymer can also be improved by adding 0.3% Attagel-50 and 0.5% polypropylene fiber by mass at a temperature of 20 °C to cope with the changeable environmental conditions on the Moon. After curing under a simulated lunar environment, the 72-h flexural and compressive strengths of the geopolymer specimens reach 4.1 and 48.1 MPa, respectively, which are promising considering that the acceleration of gravity on the Moon is 1/6 of that on the Earth.

关键词： geopolymer     lunar regolith simulant     3D printing     rheology     printability    

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Rh<sub>2sub>O<sub>3sub>/hexagonal CePO<sub>4sub> nanocatalysts for N<sub>2sub>O decomposition

Huan Liu, Zhen Ma

《化学科学与工程前沿（英文）》 2017年 第11卷 第4期   页码 586-593 doi: 10.1007/s11705-017-1659-6

摘要： Hexagonal CePO nanorods were prepared by a precipitation method and hexagonal CePO nanowires were prepared by hydrothermal synthesis at 150 °C. Rh(NO ) was then used as a precursor for the impregnation of Rh O onto these CePO materials. The Rh O supported on the CePO nanowires was much more active for the catalytic decomposition of N O than the Rh O supported on CePO nanorods. The stability of both catalysts as a function of time on stream was studied and the influence of the co-feed (CO , O , H O or O /H O) on the N O decomposition was also investigated. The samples were characterized by N adsorption-desorption, inductively coupled plasma optical emission spectroscopy, X-ray diffraction, transmission electron microscopy, X-ray photoelectron microscopy, hydrogen temperature-programmed reduction, oxygen temperature-programmed desorption, and CO temperature-programmed desorption in order to correlate the physicochemical and catalytic properties.

关键词： Rh2O3     CePO4     N2O decomposition    

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过硫酸盐诱导的缺陷氮化碳中三配位氮（N3<sub>Csub>）空位增强光催化产过氧化氢 Article

缪蔚, 王奕杰, 刘莹, 秦贺贺, 褚成成, 毛舜

《工程（英文）》 2023年 第25卷 第6期   页码 214-221 doi: 10.1016/j.eng.2021.12.016

摘要： 其中石墨氮化碳（g-C<sub>3sub>N<sub>4sub>）被认为是最有前途的合成过氧化氢的光催化剂之一；并且，在g-C<sub>3sub>N<sub>4sub>中引入氮空位已被证明是提高其光催化活性的有效策略在此，本文提出了一种简便的过硫酸钠共晶聚合方法，制备了具有丰富三配位氮空位（N3<sub>Csub>）的g-C<sub>3sub>N<sub>4sub>。本研究的结果表明，在g-C<sub>3sub>N<sub>4sub>中引入N3<sub>Csub>空位可以成功地拓宽光吸收范围，抑制光激发电荷的重组，增强O<sub>2sub>的吸附和活化富含N3<sub>Csub>空位的g-C<sub>3sub>N<sub>4sub>的光催化过氧化氢产量是原始g-C<sub>3sub>N<sub>4sub>的4.5倍。本研究提出了在g-C<sub>3sub>N<sub>4sub>中引入N3<sub>Csub>空位的新策略，为开发光催化产过氧化氢的活性催化剂提供了一种新方法。

关键词： 氮化碳     N3<sub>Csub>空位     过氧化氢     光催化     过硫酸盐    

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含稀释剂的Al-Cr<sub>2sub>O<sub>3sub>体系燃烧合成反应热力学分析与反应模型

张衍诚,潘冶,张传

《中国工程科学》 2004年 第6卷 第6期   页码 63-67

摘要：

对含稀释剂Al203和Cr<sub>2</sub>0<sub>3</sub>的Al-Cr<sub>2</sub>0<sub>3</sub>体系燃烧合成反应进行了热力学计算与分析，讨论了起始反应温度T<sub>0</sub>、稀释剂Al<sub>2</sub>O<sub>3</sub>和Cr<sub>2</sub>O<sub>3</sub>的含量对绝热反应温度7^的影响，并得出T<sub>0</sub>与T<sub>ad</sub>在特定温度段上的近似线性关系以及该关系在指导材料成分设计上的应用；揭示了反应驱动力—&mdash

关键词： 金属陶瓷     燃烧合成     Al-Cr203体系     热力学     反应模型    

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In-MOF-derived In<sub>2sub>S<sub>3sub>/Bi<sub>2sub>S<sub>3sub> heterojunction for enhanced photocatalytic

《能源前沿（英文）》 2023年 第17卷 第5期   页码 654-663 doi: 10.1007/s11708-023-0885-5

摘要： Transition metal sulfides are commonly studied as photocatalysts for water splitting in solar-to-fuel conversion. However, the effectiveness of these photocatalysts is limited by the recombination and restricted light absorption capacity of carriers. In this paper, a broad spectrum responsive In2S3/Bi2S3 heterojunction is constructed by in-situ integrating Bi2S3 with the In2S3, derived from an In-MOF precursor, via the high-temperature sulfidation and solvothermal methods. Benefiting from the synergistic effect of wide-spectrum response, effective charge separation and transfer, and strong heterogeneous interfacial contacts, the In2S3/Bi2S3 heterojunction demonstrates a rate of 0.71 mmol/(g∙h), which is 2.2 and 1.7 times as much as those of In2S3 (0.32 mmol/(g∙h) and Bi2S3 (0.41 mmol/(g∙h)), respectively. This paper provides a novel idea for rationally designing innovative heterojunction photocatalysts of transition metal sulfides for photocatalytic hydrogen production.

关键词： photocatalytic hydrogen production     wide-spectrum response     metal sulfides     MOFs derivative     heterogeneous interfacial contact    

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The stabilization effect of Al<sub>2sub>O<sub>3sub> on unconventional Pb/SiO<sub>2sub> catalyst

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1423-1429 doi: 10.1007/s11705-023-2315-y

摘要： Similar to Sn, Pb located at the same group (IVA) in the periodic table of elements, can also catalyze propane dehydrogenation to propene, while a fast deactivation can be observed. To enhance the stability, the traditional carrier Al2O3 with a small amount, was introduced into Pb/SiO2 catalyst in this study. It has been proved that Al2O3 can inhibit the reduction of PbO, and weaken the agglomeration and loss of Pb species due to its enhanced interaction with Pb species. As a result, 3Al15Pb/SiO2 catalyst exhibits a much higher stability up to more than 150 h. In addition, a simple schematic diagram of the change of surface species on the catalyst surface after Al2O3 addition was also proposed.

关键词： Pb/SiO2     Al2O3     propane dehydrogenation     propene     stability    

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acid anions on highly efficient Ce-based catalysts for selective catalytic reduction of NO with NH<sub>3sub>

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1399-1411 doi: 10.1007/s11705-023-2345-5

摘要： Three kinds of Ce-based catalysts (CePO4, CeVO4, Ce2(SO4)3) were synthesized and used for the selective catalytic reduction (SCR) of NO by NH3. NH3-SCR performances were conducted in the temperature range of 80 to 400 °C. The catalytic efficiencies of the three catalysts are as follow: CePO4 > CeVO4 > Ce2(SO4)3, which is in agreement with their abilities of NH3 adsorption capacities. The highest NO conversion rate of CePO4 could reach about 95%, and the catalyst had more than 90% NO conversion rate between 260 and 320 °C. The effect of PO43–, VO43– and SO42– on NH3-SCR performances of Ce-based catalysts was systematically investigated by the X-ray photoelectron spectroscopy analysis, NH3 temperature programmed desorption, H2 temperature programmed reduction and field emission scanning electron microscopy tests. The key factors that can enhance the SCR are the existence of Ce4+, large NH3 adsorption capacity, high and early H2 consumptions, and suitable microstructures for gas adsorption. Finally, CePO4 and CeVO4 catalysts also exhibited relatively strong tolerance of SO2, and the upward trend about 8% was detected due to the sulfation enhancement by SO2 for Ce2(SO4)3.

关键词： CePO4     CeVO4     Ce2(SO4)3     selective catalytic reduction     NO removal    

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On the monolayer dispersion behavior of Co<sub>3sub>O<sub>4sub> on HZSM-5 support: designing applicable

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1741-1754 doi: 10.1007/s11705-023-2332-x

摘要： Based on monolayer dispersion theory, Co3O4/ZSM-5 catalysts with different loadings have been prepared for selective catalytic reduction of nitrogen oxides by ammonia. Co3O4 can spontaneously disperse on HZSM-5 support with a monolayer dispersion threshold of 0.061 mmol 100 m–2, equaling to a weight percentage around 4.5%. It has been revealed that the quantities of surface active oxygen (O2–) and acid sites are crucial for the reaction, which can adsorb and activate NOx and NH3 reactants effectively. Below the monolayer dispersion threshold, Co3O4 is finely dispersed as sub-monolayers or monolayers and in an amorphous state, which is favorable to generate the two kinds of active sites, hence promoting the performance of ammonia selective catalytic reduction of nitrogen oxide. However, the formation of crystalline Co3O4 above the capacity is harmful to the reaction performance. 4% Co3O4/ZSM-5, the catalyst close to the monolayer dispersion capacity, possesses the most abundant active O2– species and acidic sites, thereby demonstrating the best reaction performance in all the samples. It is proposed the optimal Co3O4/ZSM-5 catalyst can be prepared by loading the capacity amount of Co3O4 onto HZSM-5 support.

关键词： Co3O4/ZSM-5     NOx-SCR by NH3     monolayer dispersion threshold effect     surface acid sites     surface active O2– anions    

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CO<sub>2sub> methanation and co-methanation of CO and CO<sub>2sub> over Mn-promoted Ni/Al<sub>2sub>O<sub>3sub> catalysts

Kechao Zhao,Zhenhua Li,Li Bian

《化学科学与工程前沿（英文）》 2016年 第10卷 第2期   页码 273-280 doi: 10.1007/s11705-016-1563-5

摘要： A series of Mn-promoted 15 wt-% Ni/Al O catalysts were prepared by an incipient wetness impregnation method. The effect of the Mn content on the activity of the Ni/Al O catalysts for CO methanation and the co-methanation of CO and CO in a fixed-bed reactor was investigated. The catalysts were characterized by N physisorption, hydrogen temperature-programmed reduction and desorption, carbon dioxide temperature-programmed desorption, X-ray diffraction and high-resolution transmission electron microscopy. The presence of Mn increased the number of CO adsorption sites and inhibited Ni particle agglomeration due to improved Ni dispersion and weakened interactions between the nickel species and the support. The Mn-promoted 15 wt-% Ni/Al O catalysts had improved CO methanation activity especially at low temperatures (250 to 400 °C). The Mn content was varied from 0.86% to 2.54% and the best CO conversion was achieved with the 1.71Mn-Ni/Al O catalyst. The co-methanation tests on the 1.71Mn-Ni/Al O catalyst indicated that adding Mn markedly enhanced the CO methanation activity especially at low temperatures but it had little influence on the CO methanation performance. CO methanation was more sensitive to the reaction temperature and the space velocity than the CO methanation in the co-methanation process.

关键词： Mn promotion     nickel catalysts     CO2 methanation     co-methanation of CO and CO2    

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Is atmospheric oxidation capacity better in indicating tropospheric O formation?

《环境科学与工程前沿（英文）》 2022年 第16卷 第5期 doi: 10.1007/s11783-022-1544-5

摘要：

● This study summarizes and evaluates different approaches that indicate O3 formation.

关键词： O3     AOC     O3 formation regime    

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标题 作者 时间 类型 操作

Superior performance in visible-light-driven hydrogen evolution reaction of three-dimensionally orderedmacroporous SrTiO decorated with ZnCdS

期刊论文

Fabrication of three-dimensional porous La-doped SrTiO3 microspheres with enhanced visible light catalytic

Dong Yang, Xiaoyan Zou, Yuanyuan Sun, Zhenwei Tong, Zhongyi Jiang

期刊论文

Function-reversible facets enabling SrTiO nanocrystals for improved photocatalytic hydrogen evolution

期刊论文

Enhanced photocatalytic water splitting with surface defective SrTiO

Junying LIU, Zhidong WEI, Wenfeng SHANGGUAN

期刊论文

Real drive cycles analysis by ordered power methodology applied to fuel consumption, CO

Pol Masclans Abelló, Vicente Medina Iglesias, M. Antonia de los Santos López, Jesús Álvarez-Flórez

期刊论文

Printability and hardening performance of three-dimensionally-printed geopolymer based on lunar regolith

期刊论文

Rh<sub>2sub>O<sub>3sub>/hexagonal CePO<sub>4sub> nanocatalysts for N<sub>2sub>O decomposition

Huan Liu, Zhen Ma

期刊论文

过硫酸盐诱导的缺陷氮化碳中三配位氮（N3<sub>Csub>）空位增强光催化产过氧化氢

缪蔚, 王奕杰, 刘莹, 秦贺贺, 褚成成, 毛舜

期刊论文

含稀释剂的Al-Cr<sub>2sub>O<sub>3sub>体系燃烧合成反应热力学分析与反应模型

张衍诚,潘冶,张传

期刊论文

In-MOF-derived In<sub>2sub>S<sub>3sub>/Bi<sub>2sub>S<sub>3sub> heterojunction for enhanced photocatalytic

期刊论文

The stabilization effect of Al<sub>2sub>O<sub>3sub> on unconventional Pb/SiO<sub>2sub> catalyst

期刊论文

acid anions on highly efficient Ce-based catalysts for selective catalytic reduction of NO with NH<sub>3sub>

期刊论文

On the monolayer dispersion behavior of Co<sub>3sub>O<sub>4sub> on HZSM-5 support: designing applicable

期刊论文

CO<sub>2sub> methanation and co-methanation of CO and CO<sub>2sub> over Mn-promoted Ni/Al<sub>2sub>O<sub>3sub> catalysts

Kechao Zhao,Zhenhua Li,Li Bian

期刊论文

Is atmospheric oxidation capacity better in indicating tropospheric O formation?

期刊论文