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Significantly enhanced charge transfer efficiency and surface reaction on NiP_(2)/g-C_(3)N_(4) heterojunction for photocatalytic hydrogen evolution 被引量:2
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作者 Xiaoqing Yan hua an +1 位作者 Zihao Chen Guidong Yang 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2022年第3期31-39,共9页
In this work,a novel NiP_(2)/g-C_(3)N_(4)heterojunction via homogeneous precipitation method assisted by thermal phosphorization reaction was designed and constructed,and the optimized sample showed the excellent phot... In this work,a novel NiP_(2)/g-C_(3)N_(4)heterojunction via homogeneous precipitation method assisted by thermal phosphorization reaction was designed and constructed,and the optimized sample showed the excellent photocatalytic H_(2)evolution activity under visible-light irradiation,which was nearly 112 times higher than that of pristine g-C_(3)N_(4)sample.Experimental characterizations and DFT calculations demonstrated that the NiP_(2)nanoparticles covered on the g-C_(3)N_(4)surface can form a built-in electric field at the interface to accelerate the transfer of photoexcited electrons from g-C_(3)N_(4)to NiP_(2),crucial for hindering the recombination of electron-hole pairs.Moreover,the energy barrier of hydrogen evolution reaction can also vastly reduce when combined NiP_(2)and g-C_(3)N_(4)to construct NiP_(2)/g-C_(3)N_(4)heterojunction.This work represents a method through combing experimental and theoretical tools to thoroughly investigate the mechanism of photocatalytic process. 展开更多
关键词 Carbon neutrality Charge transfer Internal electric field Photocatalytic H_(2)generation
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SiC/Pt/CdS纳米棒Z型异质结的制备及其高效光催化产氢性能 被引量:14
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作者 曹丹 安华 +3 位作者 严孝清 赵宇鑫 杨贵东 梅辉 《物理化学学报》 SCIE CAS CSCD 北大核心 2020年第3期93-106,共14页
本文采用简单的化学还原辅助水热法制备了一种新型Si C/Pt/Cd SZ型异质结纳米棒,并将Pt纳米粒子锚定在Si C纳米棒与Cd S纳米粒子的界面间,诱导电子-空穴对沿着Z型迁移路径进行转移。进行一系列的表征来分析该催化体系的结构,形貌和性能... 本文采用简单的化学还原辅助水热法制备了一种新型Si C/Pt/Cd SZ型异质结纳米棒,并将Pt纳米粒子锚定在Si C纳米棒与Cd S纳米粒子的界面间,诱导电子-空穴对沿着Z型迁移路径进行转移。进行一系列的表征来分析该催化体系的结构,形貌和性能。X射线衍射(XRD)和X射线光电子能谱(XPS)结果表明,成功合成了具有较好晶体结构的光催化剂。通过透射电子显微镜证明,Pt纳米颗粒生长在Si C纳米棒和Cd S纳米颗粒的界面间。UV-Vis漫反射光谱显示,所制备的Z-型异质结样品具有比原始Cd S材料更宽的光吸收范围。光致发光光谱和瞬态光电流响应进一步证明具有最佳摩尔比的Si C/Pt/Cd S纳米棒样品具有最高的电子-空穴对分离效率。通过控制Si C和Cd S的摩尔比,可以有效地调节Si C/Pt纳米棒表面Cd S的负载量,从而使得Si C/Pt/Cd S纳米棒光催化剂达到最佳性能。当Si C:Cd S=5:1(摩尔比)时可以达到最佳产氢性能,其最大析氢速率达到122.3μmol·h-1。此外,从扫描电子显微镜、XRD和XPS分析可以看出,经过三次循环测试后,Si C/Pt/Cd S光催化剂的形貌和晶体结构均基本保持不变,表明Si C/Pt/Cd S纳米复合材料在可见光下产氢时具有稳定的结构。通过选择性光沉积技术在光反应中同时进行Au纳米粒子的光还原沉积和Mn3O4纳米粒子光氧化沉积以证明电子-空穴对的Z-型转移机制。实验结果表明,Cd S导带上的电子主要参与光催化过程中的还原反应,Si C价带上的空穴更容易发生氧化反应,其中,Si C的导带上的电子将与Cd S价带上的空穴复合形成Z型传输路径。因此,提出了在光催化产氢过程中Si C/Pt/Cd S纳米棒催化体系可能的Z-型电荷迁移路径来解释产氢活性的提高。该研究为基于Si C纳米棒的Z-型光催化体系的合成提供了新的策略。基于以上分析,Si C/Pt/Cd S纳米复合材料具有高效、廉价、易于制备、结构稳定等优势,具有突出的商业应用前景。 展开更多
关键词 碳化硅 纳米棒 SiC/Pt/CdS 光催化剂 Z型异质结
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Nitrogen removal characteristics of heterotrophic nitrification-aerobic denitrification by Alcaligenes faecalis C16 被引量:27
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作者 Yuxiang Liu Yao Wang +2 位作者 Yi Li hua an Yongkang Lv 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2015年第5期827-834,共8页
Alcaligenes faecalis C16 was found to have the ability to heterotrophically nitrify and aerobically denitrify. In order to further understand its nitrogen removal ability and mechanism, the growth and ammonium removal... Alcaligenes faecalis C16 was found to have the ability to heterotrophically nitrify and aerobically denitrify. In order to further understand its nitrogen removal ability and mechanism, the growth and ammonium removal response were investigated at different C/N ratios and ammonium concentrations in the medium with citrate and acetate as carbon source separately. Furthermore, experiments of nitrogen sources, production of nitrogen gas and enzyme assay were conducted. Results show that the bacterium converts NH+4-N and produces NH2 OH during the growing phase and nitrite accumulation is its distinct metabolic feature. A. faecalis C16 is able to tolerate not only high ammonium concentration but also high C/N ratio, and the ammonium tolerance is associated with carbon source and C/N ratio. The nitrogen balance under different conditions shows that approximately28%–45% of the initial ammonium is assimilated into the cells, 44%–60% is denitrified and several percent is converted to nitrification products. A. faecalis C16 cannot utilize hydroxylamine, nitrite or nitrate as the sole nitrogen source for growth. However, nitrate can be used when ammonium is simultaneously present in the medium. A possible pathway for nitrogen removal by C16 is suggested. The preliminary enzyme assay provides more evidence for this nitrogen removal pathway. 展开更多
关键词 异养硝化 粪产碱菌 脱氮 好氧 反硝化 亚硝酸盐 特性 生长阶段
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新型BiOI/g-C_3N_4纳米片复合光催化剂的制备及其可见光催化活性增强(英文) 被引量:16
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作者 安华 林波 +4 位作者 薛超 严孝清 代艳竹 魏进家 杨贵东 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第4期654-663,共10页
近年来,石墨型氮化碳(g-C_3N_4)作为一种n型半导体光催化剂材料,由于具有较好的热稳定性和化学稳定性,同时具有可调的带隙结构和优异的表面性质而备受人们关注.然而,传统的g-C_3N_4块体材料存在比表面积小、光响应范围窄和光生载流子易... 近年来,石墨型氮化碳(g-C_3N_4)作为一种n型半导体光催化剂材料,由于具有较好的热稳定性和化学稳定性,同时具有可调的带隙结构和优异的表面性质而备受人们关注.然而,传统的g-C_3N_4块体材料存在比表面积小、光响应范围窄和光生载流子易复合等缺陷,制约着其光催化活性的进一步提高.因此,人们开发了多种技术对块体状g-C_3N_4材料进行改性,其中构建基于g-C_3N_4纳米薄片的异质结复合光催化材料被认为是强化g-C_3N_4载流子分离效率,进而提高其可见光催化活性的重要手段.BiOI作为一种窄带隙的p型半导体光催化剂,具有强的可见光吸收能力和较高的光催化活性,同时它与g-C_3N_4纳米薄片具有能级匹配的带隙结构.因此,基于以上两种半导体材料的特性,构建新型的BiOI/g-C_3N_4纳米片复合光催化剂材料不仅能够有效提高g-C_3N_4的可见光利用率,而且还可以在n型g-C_3N_4和p型BiOI界面间形成内建电场,极大促进光生电子-空穴对的分离与迁移效率.为此,本文通过简单的一步溶剂热法在g-C_3N_4纳米薄片表面原位生长BiOI纳米片材料,成功制备了新型的BiOI/g-C_3N_4纳米片复合光催化剂.利用X射线衍射仪(XRD),场发射扫描电子显微镜(SEM)、透射电子显微镜(TEM)、紫外-可见漫反射光谱和瞬态光电流响应谱对所合成复合光催化剂的晶体结构、微观形貌、光吸收性能和电荷分离性能进行了表征测试.XRD,SEM和TEM结果显示,结晶完好的BiOI呈小片状均匀分散在g-C_3N_4纳米薄片表面;紫外漫反射光谱表明,纳米片复合材料的吸光性能较g-C_3N_4薄片有显著提升;瞬态光电流测试证明,复合材料较单一材料有更好的电荷分离与迁移性能.在可见光催化降解RhB的测试中,BiOI/g-C_3N_4纳米片复合光催化剂显示出了优异的催化活性和稳定性,其光降解活性分别为纯BiOI和g-C_3N_4的34.89和1.72倍;自由基捕获实验发现,反应过程中的主要活性物种为超氧自由基(·O_2^-),即光生电子主导整个降解反应的发生.由此可见,强的可见光吸收能力和g-C_3N_4与BiOI界面处形成的内建电场协同促进了g-C_3N_4纳米薄片的电荷分离,进而显著提高了该复合材料的可见光催化降解活性.此外,本文初步验证了在BiOI/g-C_3N_4纳米片复合光催化体系内光生电荷是依据"双向转移"机制进行分离和迁移的,而非"Z型转移"机制. 展开更多
关键词 g-C3N4 BiOI 纳米片 光降解 双向转移 可见光
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源于功函数差异的界面内建电场调控载流子定向分离的作用机制研究 被引量:2
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作者 薛超 安华 +1 位作者 邵国胜 杨贵东 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第4期583-594,共12页
近年来,由有机污染物和重金属引起的水污染对人类健康、生态系统和社会可持续发展构成了严重威胁.而光催化技术以其高效、低成本、节能、无二次污染等优点成为解决日益严重的环境污染问题的一个极具吸引力的策略.众所周知,宽光谱吸收、... 近年来,由有机污染物和重金属引起的水污染对人类健康、生态系统和社会可持续发展构成了严重威胁.而光催化技术以其高效、低成本、节能、无二次污染等优点成为解决日益严重的环境污染问题的一个极具吸引力的策略.众所周知,宽光谱吸收、高效载流子分离和快速的表面反应动力学是高性能光催化剂所必备的基本条件.而多孔TiO_(2)空心球具有以下结构优势:(1)成本低、无毒、氧化还原电位适中、物理化学性质稳定;(2)中空结构有利于入射光多重散射,而且大表面积可以暴露更多的活性位点;(3)多孔结构有利于传质过程.但是,窄光谱吸收和低的光生载流子分离效率严重阻碍了空心结构TiO_(2)的实际应用.因此,通过耦合窄带隙半导体构建异质结光催化剂可以有效提高光吸收和促进光生电荷的分离.窄带隙(Eg=2.18–2.44 eV)半导体材料SnS_(2)具有无毒、化学性质稳定、低成本和宽谱响应等诸多优点.若将超薄SnS_(2)纳米片锚定生长在多孔TiO_(2)空心球表面,将对异质结的光催化性能产生显著的影响.一方面,分级结构的空心球具有高可见光捕获率;另一方面,超薄SnS_(2)纳米片具有更短的载流子扩散距离,从而有效地抑制光生载流子在催化剂体相内部复合.然而,由于其能带结构的限制,二元TiO_(2)/SnS_(2)复合材料很容易形成嵌入式I型异质结,在很大程度上降低了光催化氧化还原能力.此外,在光催化剂表面聚集的光生电子和空穴容易发生随机性复合.因此,迫切需要通过引入界面驱动力来调节表面载流子的分离和转移.众多研究表明,通过化学功能化可以实现对还原氧化石墨烯(rGO)的能带结构、功函数、电导率、亲水性和光学性质的调控.功能化的rGO可以作为优良的空穴提取材料,在rGO两侧分别耦合不同能级结构的半导体光催化材料,通过异质界面能级和功函数差异带来的界面内建电场,精确调控光生载流子在界面间的空间分离和定向迁移.基于上述分析,本文通过改进的“硅保护煅烧”方法合成了分级多孔SnS_(2)/rGO/TiO_(2)空心球异质结光催化剂.分级多孔空心球的结构优势不仅增强其光捕获能力,而且为光氧化还原反应提供了丰富的活性位点.特别是,在TiO_(2)和SnS_(2)纳米薄片之间嵌入的rGO中间层可以作为空穴注入层.由不同功函数导致的界面内建电场可以精确地调控光生空穴从SnS_(2)纳米薄片的价带向rGO空穴注入层定向迁移,显著延长了光生载流子的寿命.在可见光照射下,负载2 wt%rGO的分级多孔SnS_(2)/rGO/TiO_(2)空心球异质结光催化剂对罗丹明B染料的降解率可达97.3%,对Cr(VI)的还原效率可达97.09%.此外,经过六个周期的循环实验,该异质结催化降解罗丹明B和还原Cr(VI)的效率没有明显降低,表现出较好的光催化稳定性. 展开更多
关键词 SnS_(2)/rGO/TiO_(2) 空心球 光催化剂 空穴注入层 CR(VI)还原
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Meniscus repair with simultaneous anterior cruciate ligament reconstruction: Clinical outcomes, failure rates and subsequent processing
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作者 Yu-Ping Yang Xiao Ma +3 位作者 hua an Xiao-Peng Liu Ning an Ying-Fang Ao 《Chinese Journal of Traumatology》 CAS CSCD 2022年第1期37-44,共8页
Purpose::To retrospectively analyze the clinical outcomes of meniscus repair with simultaneous anterior cruciate ligament(ACL)reconstruction and explore the causes of failure of meniscus repair.Methods::From May 2013 ... Purpose::To retrospectively analyze the clinical outcomes of meniscus repair with simultaneous anterior cruciate ligament(ACL)reconstruction and explore the causes of failure of meniscus repair.Methods::From May 2013 to July 2018,the clinical data of 165 patients who were treated with meniscus surgery and simultaneous ACL reconstruction,including 69 cases of meniscus repair(repair group)and 96 cases of partial meniscectomy(partial meniscectomy group)were retrospectively analyzed.The exclusion criteria were as follows:(1)ACL rupture associated with fracture,collateral ligament injury,or complex ligament injury;(2)a history of knee surgery;or(3)a significant degree of osteoarthritis.The 69 patients in the repair group were divided into the non-failure group(62 cases)and the failure group(7 cases)depending on the repair effect.Postoperative outcomes of the repair group and the partial meniscectomy group were compared.General conditions and postoperative outcomes of the failure group and the non-failure group were compared.During the median follow-up period of 28 months(range,4-65 months)after the second arthroscopy,postoperative outcomes of seven patients in the failure group were summarized.SPSS 25.0 statistical software was used for statistical analysis.A p value less than 0.05 was considered statistically significant.Results::Seven patients in the failure group who underwent the second arthroscopy were followed up for(30±17.4)months and their postoperative outcomes were summarized.Compared with the partial meniscectomy group,the International Knee Documentation Committee scores of patients in the repair group improved significantly(p=0.031).Compared with the non-failure group,more patients in the failure group were younger than 24 years(p=0.030).The median follow-up period was 39.5 months.All patients recovered well after subsequent partial meniscectomy and relieved clinical symptoms.Visual analog scale scores decreased significantly(p=0.026),and the International Knee Documentation Committee and Lysholm scores improved significantly(p=0.046 for both).Conclusion::The failure rate of meniscus repair in this study was 10.1%(7/69),all of which were medial meniscus tears.However,the surgical outcomes of ACL reconstruction were not affected,and there might be a role for graft protection.Therefore,meniscus retears can be successful treated by performing subsequent partial meniscectomy in patients with repair failure. 展开更多
关键词 MENISCUS Failure of repair Anterior cruciate ligament reconstruction ARTHROSCOPY
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从意念的革命到现实的革命——马克思对康德的继承与超越 被引量:2
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作者 华安 《马克思主义理论学科研究》 CSSCI 2019年第4期176-182,共7页
革命理论是马克思与康德之间的思想桥梁,是马克思对德国古典哲学创始人康德的继承与超越的关键一环。康德在其哲学中已经论述过有关革命的思想,只是康德所倡导的革命是一种'意念的革命';而马克思继承了这一'康德遗产',... 革命理论是马克思与康德之间的思想桥梁,是马克思对德国古典哲学创始人康德的继承与超越的关键一环。康德在其哲学中已经论述过有关革命的思想,只是康德所倡导的革命是一种'意念的革命';而马克思继承了这一'康德遗产',用'现实的革命'超越了康德,最终完善了革命理论。 展开更多
关键词 马克思 康德 革命
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Ionic Liquid-Stabilized Single-Atom Rh Catalyst Against Leaching 被引量:1
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作者 Shipeng Ding Max JHülsey +6 位作者 hua an Qian He Hiroyuki Asakura Min Gao Jun-ya Hasegawa Tsunehiro Tanaka Ning Yan 《CCS Chemistry》 CAS 2021年第10期1814-1822,共9页
Single-atom catalysts(SACs)are promising in some reactions typically promoted by homogeneous catalysts.However,the leaching of active species from the support in liquid-phase reactions hinders their potential applicat... Single-atom catalysts(SACs)are promising in some reactions typically promoted by homogeneous catalysts.However,the leaching of active species from the support in liquid-phase reactions hinders their potential applications.Herein,taking the hydroformylation reaction as an example,we report ionic liquid(IL)-induced stabilization of single Rh atoms against leaching.Among the ILs examined. 展开更多
关键词 single-atom catalysts electrostatic stab ilization ionic liquid LEACHING
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