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Design of Bi4O5Br2/g-C3N4 heterojunction for efficient photocatalytic removal of persistent organic pollutants from water 高效光催化去除水中持久性有机污染物的Bi4O5Br2/g-C3N4异质结设计
Pub Date : 2023-10-31 DOI: 10.1002/ece2.8
Pin Song, Jun Du, Xinliang Ma, Yunmei Shi, Xiaoyu Fang, Daobin Liu, Shiqiang Wei, Zhanfeng Liu, Yuyang Cao, Bo Lin, Jun Di, Yan Wang, Jiewu Cui, Tingting Kong, Chao Gao, Yujie Xiong

Dyes and antibiotics as typical persistent organic pollutants (POPs) are widely present in the environment, but can hardly be removed completely by traditional water treatment methods. Here, we designed Bi4O5Br2/g-C3N4 composite nanosheets for efficient photocatalytic removal of POPs in water. The Bi4O5Br2/g-C3N4 composite with a heterojunction structure exhibited high adsorption and photocatalytic activity for removal of tetracycline (TC) and ciprofloxacin (CIP) with excellent cyclic stability, owing to its large specific surface area as well as enhanced charge separation and visible light utilization. Our characterization revealed that h+ and ·OH are responsible for the photocatalytic degradation of TC and CIP. This work provides insights into the design of photocatalytic materials with synergy of adsorption and photocatalytic degradation, and offers a heterojunction construction strategy for addressing the increasingly severe environmental issues.

染料和抗生素作为典型的持久性有机污染物广泛存在于环境中,但传统的水处理方法很难完全去除。在这里,我们设计了Bi4O5Br2/g-C3N4复合纳米片,用于高效光催化去除水中的POPs。具有异质结结构的Bi4O5Br2/g-C3N4复合材料由于具有较大的比表面积、增强的电荷分离和可见光利用率,对四环素(TC)和环丙沙星(CIP)具有较高的吸附和光催化活性,并且具有良好的循环稳定性。我们的表征表明,h+和·OH参与了TC和CIP的光催化降解。本研究为吸附和光催化降解协同作用的光催化材料的设计提供了新的思路,并为解决日益严峻的环境问题提供了异质结的构建策略。
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引用次数: 0
Monomicelle-induced assembly route toward low-dimensional mesoporous nanomaterials for catalysis 单胶团诱导组装低维介孔纳米材料的催化途径
Pub Date : 2023-10-30 DOI: 10.1002/ece2.7
Wei Zhang, Kerun Zhu, Chaochao Yang, Yan Ai, Yihan Gao, Wei Li, Dongyuan Zhao

Low-dimensional mesoporous nanomaterials (LDMNs), which possess complementary properties in the mesoscale and nanoscale, have realized more technological potentials in a wide range of applications, in particular, catalysis. Although still in its infancy, the proposed monomicelles-induced assembly (MIA) has been proved to be an emerging and powerful toolbox for the direct synthesis of LDMNs with well-controlled mesostructures and architectures. This review starts from the developmental history of the MIA strategy and then discuss general protocols to fabricate the monomicelles. After that, manipulation of the monomicelles' assembly by well-designed interfaces and confined spaces for the controllable fabrication of LDMNs are reviewed in detail. Then, catalytic applications, including thermal, photo- and electrocatalysis, of LDMNs are discussed critically based on the structure-performance relationship. This review ends with a brief summary and further directions of the MIA strategy, paving the way for the synthesis of sophisticated mesoporous assemblies to achieve advanced functionalities.

低维介孔纳米材料(LDMNs)在介孔尺度和纳米尺度上具有互补的特性,具有广泛的应用潜力,特别是在催化方面。尽管仍处于起步阶段,但单细胞诱导组装(MIA)已被证明是直接合成具有良好介观结构和结构控制的ldmn的新兴和强大的工具箱。本文从MIA策略的发展历史出发,讨论了单束制备的一般方案。然后,通过精心设计的界面和有限空间来操纵单束组装,以实现ldmn的可控制造。然后,基于结构-性能关系,重点讨论了ldmn的催化应用,包括热催化、光催化和电催化。本文以简要总结和MIA策略的进一步方向结束,为合成复杂的介孔组装体以实现先进的功能铺平了道路。
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引用次数: 0
Nanoclusters for photoelectrochemical water splitting: Bridging the photosensitizer and carrier transporter 用于光电化学水分解的纳米团簇:桥接光敏剂和载流子转运体
Pub Date : 2023-10-30 DOI: 10.1002/ece2.6
Yonghao Xiao, Chuanhao Yao, Chenliang Su, Bin Liu

Increasing global environmental deterioration is becoming a serious concern, leading to an exponential increase in scientific interest in renewable energy as an alternative to replace fossil fuels. Photoelectrochemical (PEC) water splitting, which directly converts sunlight into hydrogen fuel, offers a promising renewable energy technology. Semiconductors, used as photoelectrodes, provide the most feasible method for converting solar energy into electrical energy and chemical fuels. Unfortunately, most of the common semiconductors used in PEC water splitting have wide bandgaps, which greatly restrict the utilization efficiency of sunlight. To promote the solar-to-hydrogen (STH) efficiency of PEC water splitting, atomically precise clusters with regular crystal structures have been introduced in the PEC systems. In this review, the recent advances in nanoclusters for PEC water splitting, including metal clusters, polyoxometalates, semiconductor clusters, and carbon clusters, are summarized. At last, major challenges and outlook for the development of clusters for PEC water splitting are provided.

日益严重的全球环境恶化正成为一个严重问题,导致科学界对可再生能源作为化石燃料替代品的兴趣呈指数级增长。光电化学(PEC)水分解技术将太阳光直接转化为氢燃料,是一种很有前途的可再生能源技术。半导体作为光电极,为将太阳能转化为电能和化学燃料提供了最可行的方法。遗憾的是,大多数用于PEC水分解的普通半导体具有较宽的带隙,这极大地限制了对太阳光的利用效率。为了提高太阳能-氢(STH)在太阳能-氢系统中的分解效率,在太阳能-氢系统中引入了具有规则晶体结构的原子精度团簇。本文综述了近年来用于PEC水分解的纳米团簇的研究进展,包括金属团簇、多金属氧酸盐团簇、半导体团簇和碳团簇。最后,提出了PEC水裂解集群发展面临的主要挑战和展望。
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引用次数: 0
Advances in hydrogen energy conversion of graphdiyne-based materials 石墨烯基材料氢能转换研究进展
Pub Date : 2023-10-20 DOI: 10.1002/ece2.5
Xuchen Zheng, Yurui Xue, Siao Chen, Yuliang Li

Graphdiyne (GDY), a new carbon allotrope containing sp and sp2-hybridized carbon atoms, features the one-atom-thick two-dimensional structure with many unique and promising characteristics, such as highly conjugated and extremely large π structures, abundant carbon chemical bonds, naturally distributed pores, inherent band gap, excellent chemical and mechanical stability, highly uneven distributed surface charges, and can be grown on the surface of arbitrary substrates. GDY has been one of the hottest frontiers in chemistry and material sciences and represents a new development trend and research direction in the development of carbon materials. Owing to the unique characteristics in chemical and electronic structures, GDY has shown great application potentials and prospects in many fields, including catalysis, energy, optoelectronics, life science, and intelligent device. In this review, the structures, synthetic methods, and fundamental properties of GDY are introduced. In particular, the recent advances of GDY and its formed aggregates in hydrogen energy conversion are summarized and discussed.

石墨炔(GDY)是一种含有sp和sp2杂化碳原子的新型碳同素异形体,具有单原子厚的二维结构,具有高共轭和超大π结构、丰富的碳化学键、自然分布的孔隙、固有的带隙、优异的化学和机械稳定性、表面电荷分布极不均匀等许多独特而有前景的特性,可以在任意基底表面生长。GDY已成为化学和材料科学的前沿热点之一,代表了碳材料发展的新趋势和研究方向。由于其独特的化学和电子结构特点,GDY在催化、能源、光电子、生命科学、智能设备等诸多领域显示出巨大的应用潜力和前景。本文介绍了GDY的结构、合成方法及基本性能。特别对GDY及其形成的聚集体在氢能转化方面的最新进展进行了总结和讨论。
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引用次数: 0
Design strategies of ruthenium-based materials toward alkaline hydrogen evolution reaction 钌基材料对碱性析氢反应的设计策略
Pub Date : 2023-10-10 DOI: 10.1002/ece2.4
Liqiang Hou, Haeseong Jang, Xiumin Gu, Xuemei Cui, Jiachen Tang, Jaephil Cho, Xien Liu

Hydrogen produced from electrocatalytic water splitting means is deemed to be a promising route to construct a low-carbon, eco-friendly, and high-efficiency modern energy system. The design and construction of highly active catalysts with affordable prices toward alkaline hydrogen evolution reaction (HER) are effective in accelerating the overall water-splitting process. So far, ruthenium (Ru) based catalysts deliver comparable or even superior catalytic performance relative to the platinum (Pt)/C benchmark. Combined with their price advantage, Ru-based catalysts are undoubtedly considered as one of the perfect alternatives of Pt toward the alkaline HER. Extensive efforts have been made to reasonably synthesize Ru-related materials, but a careful insight into material engineering strategies and induced effects remain in its infancy. In this review, recent progress on the material engineering strategies for improving the catalytic activity of Ru-related catalysts, including electronic regulation, geometric modulation, local structure alteration, self-optimization strategies, and the induced structure–activity relationship are comprehensively summarized. Furthermore, the challenges and perspectives on future studies of Ru-related electrocatalysts for the alkaline HER are also proposed.

电催化水裂解制氢被认为是构建低碳、环保、高效的现代能源体系的一条很有前途的途径。设计和构建价格合理的碱性析氢反应高活性催化剂是加速整个水裂解过程的有效手段。到目前为止,钌(Ru)基催化剂的催化性能与铂(Pt)/C基准相当,甚至更好。结合其价格优势,钌基催化剂无疑被认为是Pt替代碱性HER的理想选择之一。在合理合成钌相关材料方面已经做了大量的努力,但对材料工程策略和诱导效应的仔细洞察仍处于起步阶段。本文综述了近年来提高钌相关催化剂催化活性的材料工程策略,包括电子调控、几何调制、局部结构改变、自优化策略和诱导构效关系等方面的研究进展。最后,对碱性HER中钌相关电催化剂的研究提出了挑战和展望。
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引用次数: 1
Fabricating freestanding electrocatalyst with bismuth-iron dual active sites for efficient ammonia synthesis in neutral media 中性介质中高效合成氨用铋铁双活性位独立式电催化剂的制备
Pub Date : 2023-09-18 DOI: 10.1002/ece2.3
Ying Sun, Zhuoying Sun, Wei Zhang, Wentao Li, Chang Liu, Qin Zhao, Zihang Huang, Hui Li, Jingang Wang, Tianyi Ma

Electrocatalytic N2 reduction (NRR) has been regarded as a promising approach for environment-friendly and sustainable ammonia (NH3) synthesis. However, developing cost-effective electrocatalysts with high NRR efficiency at low overpotential in neutral media remains a great challenge. In this paper, a freestanding NRR electrocatalyst, BiFeO/FCC, has been developed by in situ growth of bismuth ferrite (Bi25FeO40) on functionalized carbon cloth (FCC), which exhibits high NRR activity with a maximum NH3 yield of 3.88 μg h−1 cm−2 (at −0.40 V vs. reversible hydrogen electrode [RHE]) and a Faradaic efficiency of 12.71% (at −0.45 V vs. RHE) in 0.1 M Na2SO4. The synergistic effect of the abundant exposed bismuth and iron dual active sites confined in the lattice, the binder-free nature of the electrode and the excellent conductivity of the carbon substrate enable the easy adsorption/activation of N2 and accelerate the electron transfer simultaneously, thus boosting its NRR performance. This work is significant to design low-cost, and high-efficient NRR catalysts for large-scale electrocatalytic NH3 synthesis.

电催化N2还原(NRR)是一种很有前途的环境友好、可持续的氨合成方法。然而,在中性介质中开发低过电位、高NRR效率的低成本电催化剂仍然是一个巨大的挑战。本文通过在功能化碳布(FCC)上原位生长铋铁氧体(Bi25FeO40),制备了一种独立的NRR电催化剂BiFeO/FCC,该催化剂具有较高的NRR活性,NH3产率最高为3.88 μg h−1 cm−2(在- 0.40 V比可逆氢电极[RHE]下),在0.1 M Na2SO4中,法拉第效率为12.71%(在- 0.45 V比RHE下)。晶格中大量暴露的铋和铁双活性位点、电极的无粘结剂性质以及碳衬底优异的导电性的协同作用,使其易于吸附/活化N2,同时加速电子转移,从而提高了其NRR性能。该工作对设计低成本、高效的NRR催化剂用于大规模电催化NH3合成具有重要意义。
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引用次数: 0
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