Bocheng Qiu

Nanjing Agricultural University

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Jinlong Zhang

Guizhou University

Mingyang Xing

East China University of Science and Technology

Yang Chai

Hong Kong Polytechnic University

Mengmeng Du

Nanjing Agricultural University

Lejuan Cai

Songshan Lake Materials Laboratory

Qiaohong Zhu

Hangzhou Normal University

Yingxin Ma

Shenzhen Institutes of Advanced Technology

Ning Zhang

Hong Kong Polytechnic University

Xuyun Guo

Trinity College Dublin

Sailei Kang

Nanjing Agricultural University

Cooperative Institutions

East China University of Science and Technology

Chinese Academy of Sciences

Hong Kong Polytechnic University

Hangzhou Normal University

University of Chinese Academy of Sciences

Nanjing Agricultural University

State Council of the People's Republic of China

Kowloon Hospital

Tsinghua University

University of Science and Technology of China

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Metal Substitution Steering Electron Correlations in Pyrochlore Ruthenates for Efficient Acidic Water Oxidation

ACS Nano (2021)

Ning Zhang Cong Wang Jiewei Chen Canyu Hu Jun Ma

Exploring the advanced oxygen evolution reaction (OER) electrocatalysts is highly desirable toward sustainable energy conversion and storage, yet improved efficiency in acidic media is largely hindered by its sluggish reaction kinetics. Herein, we rationally manipulate the electronic states of the strongly electron correlated pyrochlore ruthenate Y2Ru2O7 alternative through partial A-site substitution of Sr2+ for Y3+, efficiently improving its intrinsic OER activity. The optimized Y1.7Sr0.3Ru2O7 candidate observes a highly intrinsic mass activity of 1018 A gRu–1 at an overpotential of 300 mV with excellent durability in 0.5 M H2SO4 electrolyte. Combining synchrotron-radiation X-ray spectroscopic investigations with theoretical simulations, we reveal that the electron correlations in the Ru 4d band are weakened through coordinatively geometric regulation and charge redistribution by the exotic Sr2+ cation, enabling the delocalization of Ru 4d electrons via an insulator-to-metal transition. The induced Ru–O covalency promotion and band alignment rearrangement decreases the charge transfer energy to accelerate interfacial charge transfer kinetics. Meanwhile, the chemical affinity of oxygen intermediates is also rationalized to weaken the metal–oxygen binding strength, thus lowering the energy barrier of the overall reaction. This work offers fresh insights into designing advanced solid-state electrocatalysts and underlines the versatility of electronic structure manipulation in tuning catalytic activity.

Overpotential

Oxygen evolution

10.1021/acsnano.1c00266

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Citations (75)

Ultrathin g-C3N4 nanosheet with hierarchical pores and desirable energy band for highly efficient H2O2 production

Applied Catalysis B Environment and Energy (2019)

Liang Zhou Jianrui Feng Bocheng Qiu Yi Zhou Juying Lei

Nanosheet

Graphitic carbon nitride

10.1016/j.apcatb.2019.118396

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Citations (240)

Efficient Solar Light Harvesting CdS/Co₉S₈ Hollow Cubes for Z‐Scheme Photocatalytic Water Splitting

Angewandte Chemie International Edition (2017)

Bocheng Qiu Qiaohong Zhu Mengmeng Du Linggang Fan Mingyang Xing

Abstract Hollow structures with an efficient light harvesting and tunable interior component offer great advantages for constructing a Z‐scheme system. Controlled design of hollow cobalt sulfide (Co 9 S 8 ) cubes embedded with cadmium sulfide quantum dots (QDs) is described, using hollow Co(OH) 2 as the template and a one‐pot hydrothermal strategy. The hollow CdS/Co 9 S 8 cubes utilize multiple reflections of light in the cubic structure to achieve enhanced photocatalytic activity. Importantly, the photoexcited charge carriers can be effectively separated by the construction of a redox‐mediator‐free Z‐scheme system. The hydrogen evolution rate over hollow CdS/Co 9 S 8 is 134 and 9.1 times higher than that of pure hollow Co 9 S 8 and CdS QDs under simulated solar light irradiation, respectively. Moreover, this is the first report describing construction of a hollow Co 9 S 8 based Z‐scheme system for photocatalytic water splitting, which gives full play to the advantages of light‐harvesting and charges separation.

Cadmium sulfide

Photocatalytic water splitting

Visible spectrum

Charge carrier

10.1002/anie.201612551

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Citations (515)

A Ternary Dumbbell Structure with Spatially Separated Catalytic Sites for Photocatalytic Overall Water Splitting

Advanced Science (2020)

Bocheng Qiu Lejuan Cai Ning Zhang Xiaoming Tao Yang Chai

Solar-driven overall water splitting based on metal sulfide semiconductor photocatalysts remains as a challenge owing to the strong charge recombination and deficient catalytic active sites. Additionally, significant inhibition of back reactions, especially the oxidation of sulfide ions during the photocatalytic water oxidation catalysis, is an arduous task that requires an efficient photogenerated hole transfer dynamics. Here, a ternary dumbbell-shaped catalyst based on RuO2/CdS/MoS2 with spatially separated catalytic sites is developed to achieve simultaneous production of hydrogen and oxygen under simulated solar-light without any sacrificial agents. Particularly, MoS2 nanosheets anchored on the two ends of CdS nanowires are identified as a reduction cocatalyst to accelerate hydrogen evolution, while RuO2 nanoparticles as an oxidation cocatalyst are deposited onto the sidewalls of CdS nanowires to facilitate oxygen evolution kinetics. The density functional theory simulations and ultrafast spectroscopic results reveal that photogenerated electrons and holes directionally migrate to MoS2 and RuO2 catalytic sites, respectively, thus achieving efficient charge carrier separation. The design of ternary dumbbell structure guarantees metal sulfides against photocorrosion and thus extends their range in solar water splitting.

Dumbbell

Oxygen evolution

Photocatalytic water splitting

10.1002/advs.201903568

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Citations (129)

Trash to Treasure: Photoreforming of Plastic Waste into Commodity Chemicals and Hydrogen over MoS₂-Tipped CdS Nanorods

ACS Catalysis (2022)

Mengmeng Du Yu Zhang Sailei Kang Xuyun Guo Yingxin Ma

Plastic valorization presents a significantly untapped opportunity to address environmental issues while creating the necessary economic push for a circular carbon economy. Compared with the conventional routes for processing plastics (e.g., pyrolysis and gasification), a photoreforming strategy, namely, photocatalytic plastic oxidation paired with water splitting, aims to achieve plastic valorization into commodity chemicals under mild conditions while offering hydrogen fuels. Here, we implement MoS2-tipped CdS nanorod photocatalysts in an aqueous medium to reform pretreated plastics that range from polyesters (e.g., polylactic acid (PLA) and polyethylene terephthalate (PET)) to polyolefins (e.g., polyethylene (PE)). The architecture of MoS2/CdS takes advantage of the anisotropic morphology and rapid charge transfer features of nanorods, by collecting the electrons at the MoS2 tip for hydrogen evolution and utilizing the entire sidewall of CdS nanorods with rich holes toward plastic oxidation. It is shown that continuous H2 can be evolved from photoreforming of PLA, PET (commercial PET granules and real-world PET bottles), and PE, while these plastic substrates are accordingly converted into a series of valuable chemicals. This work provides an effective way to harness solar energy to realize the transformation of trash (plastics) to treasure (gaseous/liquid chemicals).

Nanorod

Polylactic Acid

Plastic Waste

10.1021/acscatal.2c03605

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Citations (120)

Ultrasound‐Assisted Emulsification–Microextraction Combined with Graphite Furnace Atomic Absorption Spectrometry for the Determination of Trace Lead in Water

CLEAN - Soil Air Water (2012)

Hongmei Jiang Yu Zhang Bocheng Qiu Wenhua Li

Abstract The ultrasound‐assisted emulsification–microextraction (USAEME) method was combined with graphite furnace atomic absorption spectrometry (GFAAS) for the determination of trace Pb using dithizone (H 2 DZ) as chelating reagent. Some effective parameters influenced the detection and microextraction, such as ashing temperature and atomization temperature, pH, extraction solvent, sample volume, extraction time, and extraction temperature were selected and optimized. After extraction, the calibration curves for Pb was in the concentration range of 0.1–10 ng mL −1 , and the linear equation was y = 0.097 x + 0.023 ( R = 0.99). Under the optimized conditions, the detection limit of the method was 20 pg mL −1 with an enrichment factor of 70 and the relative standards deviation (RSD) for seven determinations of 1 ng mL −1 Pb was 11%. The proposed method was successfully applied to determine trace Pb in Yueya Lake water, pond water, and spiked samples. Furthermore, a certified reference material of Environment Water (GBW08607) was analyzed and the determined value was in good agreement with the certified value, which showed the accuracy, recovery, and applicability of the reported method.

Certified reference materials

Ashing

Enrichment factor

Dithizone

10.1002/clen.201100343

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Citations (14)

Recent advances in three-dimensional graphene based materials for catalysis applications

Chemical Society Reviews (2018)

Bocheng Qiu Mingyang Xing Jinlong Zhang

Over the past few decades, two-dimensional graphene based materials (2DGMs) have piqued the interest of scientists worldwide, and the exploration of their potential applications in catalysis, sensors, electronic devices and energy storage due to their extraordinary physical and chemical properties has rapidly progressed. As for these 2DGMs, there is a complementary need to assemble 2D building blocks hierarchically into more complicated and hierarchical three-dimensional graphene-based materials (3DGMs). Such a capability is vitally crucial in order to design sophisticated and multi-functional catalysts with tailorable properties. This comprehensive review describes some important recent advances with respect to 3DGMs, including their preparation methods, characterization and applications in catalysis, e.g., photocatalysis, electrocatalysis, organic catalysis, and CO oxidation. The importance of the relationship between the structure and catalytic performance, a topic which has become a central focus of research in order to develop high-performance catalytic systems, is discussed. Likely future developments and their associated challenges are proposed and discussed.

10.1039/c7cs00904f

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Citations (450)

Facile synthesis of the Ti3+ self-doped TiO2-graphene nanosheet composites with enhanced photocatalysis

Scientific Reports (2015)

Bocheng Qiu Yi Zhou Yunfei Ma Xiaolong Yang Weiqin Sheng

This study developed a facile approach for preparing Ti(3+) self-doped TiO2-graphene photocatalyst by a one-step vacuum activation technology involved a relative lower temperature, which could be activated by the visible light owing to the synergistic effect among Ti(3+) doping, some new intersurface bonds generation and graphene oxide reduction. Compared with the traditional methods, the vacuum activation involves a low temperature and low-costing, which can achieve the reduction of GO, the self doping of Ti(3+) in TiO2 and the loading of TiO2 nanoparticles on GR surface at the same time. These resulting TiO2-graphene composites show the high photodegradation rate of MO, high hydrogen evolution activity and excellent IPCE in the visible light irradiation. The facile vacuum activation method can provide an effective and practical approach to improve the performance of TiO2-graphene and other metal oxides-graphene towards their practical photocatalytic applications.

Photodegradation

Nanosheet

Nanomaterials

Visible spectrum

10.1038/srep08591

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Citations (263)

Nickel Boride Cocatalyst Boosting Efficient Photocatalytic Hydrogen Evolution Reaction

Industrial & Engineering Chemistry Research (2018)

Qiaohong Zhu Bocheng Qiu Mengmeng Du Mingyang Xing Jinlong Zhang

Noble metals have been extensively used as catalyst promoters to driven highly efficient photocatalytic hydrogen evolution reaction (HER). However, noble-metal-based promoters are limited by their expensive costs and scarcities. Recently, massive efforts have been focused on metal phosphides, metal sulfides, and metal carbides as cocatalysts to achieve high HER performance. Currently, metal borides were reported as promoters for hydrogen evolution. Here, we demonstrate amorphous nickel boride (NiB) with a suitable band gap prepared by the chemical reduction of nickel nitrate hexahydrate using sodium borohydride as a cocatalyst over graphite carbon nitride (C3N4), thus achieving higher hydrogen evolution performance than C3N4. With the B(δ−)–Ni(δ+)–N(δ−) bonds between NiB and C3N4, the as-prepared C3N4/NiB7.5 shows a dramatically enhanced photocatalytic hydrogen generation rate (464.4 μmol h–1 g–1), and reaches a quantum efficiency of 10.92% with 365 nm light irradiation.

Sodium borohydride

Noble metal

10.1021/acs.iecr.8b01376

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Citations (63)

Spin state engineering of spinel oxides by integration of Cr doping and a p–n junction for water oxidation

Chemical Communications (2022)

Yingxin Ma Yu Zhang Mengyuan Xing Sailei Kang Mengmeng Du

Spinel Co3O4 has emerged as a promising electrocatalyst towards alkaline water oxidation, but its activity is restricted by the undesirable electronic configuration of the octahedral Co3+ site. Herein, we simultaneously manipulate Cr doping and p-n junction engineering on Co3O4 nanorods, which contributes to the formation of Co2+ and Ni3+ octahedral sites with optimal eg fillings, thus achieving a superior OER performance.

Nanorod

Oxidation state

Spin states

10.1039/d2cc02175g

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Citations (21)