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Corrigendum to “Spinel-covered interlayer MgO enhances the performance of BiVO 4 photocatalytic ammonia synthesis” [Appl. Catal. B Environ. Energy 344 (2024) 123670]

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Applied Catalysis B: Environment and Energy 2024年 348卷

作者： Kaiyi Chen Rongling Wang Qiong Mei Fei Ding Hui Liu Guidong Yang Bo Bai Qizhao Wang School of Water and Environment Key Laboratory of Subsurface Hydrology and Ecological Effects in Arid Region of Ministry of Education Key Laboratory of Subsurface Hydrology and Ecological Effect in Arid Region of the Ministry of Education Chang'an University Xi'an 710054 China School of Metallurgy and Environment Chinese National Engineering Research Center for Control & Treatment of Heavy Metal Pollution Central South University Changsha 410083 China School of Chemical Engineering and Technology Xi’an Jiaotong University Xi’an Shaanxi 710049 China College of Chemistry and Chemical Engineering Northwest Normal University Lanzhou 730070 Gansu China

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Uranium sequestration in sediment at an iron-rich contaminated site at Oak Ridge, Tennessee *** followed by reoxidation

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Journal of Environmental Sciences 2019年第11期31卷 156-167页

作者： Peng-Song Li Wei-Min Wu Debra H.Phillips David B.Watson Shelly Kelly Bing Li Tonia Mehlhorn Kenneth Lowe Jennifer Earles Hu-Chun Tao Tong Zhang Craig S.Criddle Department of Civil and Environmental Engineering William & Cloy Codiga Resource Recovery Center Center for Sustainable Development & Global Competitiveness Stanford University Stanford CA 94305-4020 USA Key Laboratory for Heavy Metal Pollution Control and Reutilization School of Environment and Energy Peking University Shenzhen Graduate School Shenzhen 518055 China Institute of New Energy Technology Tsinghua University Beijing 100084 China School of Natural and Built Environment Queen's University Belfast Belfast BT9 5AG Northern Ireland UK Environmental Sciences Division Oak Ridge National Laboratory Oak Ridge P.O.Box 2008 TN 37831 USA EXAFS Analysis Bolingbrook IL 60440 USA Department of Civil Engineering The University of Hong Kong Hong Kong China

This study evaluated uranium sequestration performance in iron-rich (30 g/kg) sediment via bioreduction followed by *** tests (1383 days) at Oak Ridge,Tennessee demonstrated that uranium contents in sediments increased after bioreduced sediments were re-exposed to nitrate and oxygen in contaminated *** of contaminated sediments (1200 mg/kg U) with ethanol in microcosm reduced aqueous U from 0.37 to 0.023 mg/*** of the bioreduced sediment were reoxidized with O2,H2O2,and NaNO3,respectively,over 285 days,resulting in aqueous U of 0.024,1.58 and 14.4 mg/L at pH 6.30,6.63 and 7.62,*** source-and the three reoxidized sediments showed different desorption and adsorption behaviors of U,but all fit a Freundlich *** adsorption capacities increased sharply at pH 4.5 to 5.5,plateaued at pH 5.5 to 7.0,then decreased sharply as pH increased from 7.0 to *** O2-reoxidized sediment retained a lower desorption efficiency at pH over *** NO3--reoxidized sediment exhibited higher adsorption capacity at pH 5.5 to *** pH-dependent adsorption onto Fe(Ⅲ) oxides and formation of U coated particles and precipitates resulted in U sequestration,and bioreduction followed by reoxidation can enhance the U sequestration in sediment.

关键词： Sediments Uranium Sequestration Bioreduction Reoxidation

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High-Throughput DFT-Assisted Design of Electrode for Efficient High-Temperature Electrochemical Dehydrogenation

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Angewandte Chemie 2025年第24期137卷

作者： Xuepeng Xiang Zilin Ma Jun Zhang Yifeng Li Yongjian Ye Wenyu Lu Mengzhen Zhou Shasha Huang Haijun Fu Bo Yu Shijun Zhao Zhang Lin Yan Chen School of Environment and Energy Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling South China University of Technology Guangzhou 510006 P.R. China Department of Mechanical Engineering City University of Hong Kong Hong Kong 999077 P.R. China SINOPEC (Beijing) Research Institute of Chemical Industry Co. Ltd Beijing 100013 P.R. China Institute of Nuclear and New Energy Technology Tsinghua University Beijing 100084 P.R. China Chinese National Engineering Research Center for Control & Treatment of Heavy Metal Pollution School of Metallurgy and Environment Central South University Changsha 410083 P.R. China

Protonic ceramic electrolysis cell (PCEC) is a promising technique to enable efficient dehydrogenation reactions for producing valuable chemicals, but is still limited by the lack of stable electrocatalysts to achieve efficient O─H/C─H dissociation. In this work, upon high-throughput first-principles calculations, Ba(Zr,Co,Fe,M)O 3 -based (M represents dopants) perovskite is formulated, and oxygen vacancy formation energy ( ) and hydration energy (Δ E hydr ) are taken as two key performance indicators to screen potential PCEC electrode materials derived from this category. Trivalent doping elements, particularly Y, Yb, Er, and Tm, achieve a good balance between and Δ E hydr . Experiments further validate that the BaZr 0.125 Co 0.375 Fe 0.375 Tm 0.125 O 3−δ showed impressive dehydrogenation reaction activity, with faradaic efficiency as high as 98.90% in water electrolysis, and outstanding ethane conversion rate (67.60%) and ethylene yield (62.62%) for ethane dehydrogenation reaction at 700 °C. The computational approach can be applied to the rational design of novel electrode materials for other electrochemical reactions in energy and environment devices.

关键词： Air electrode Barium zirconate Density functional theory Electrochemical dehydration Protonic ceramic electrochemical cells

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Achieving High Solid–Liquid Ratio through Competitive Coordination towards Efficient Recovery of metals from Spent Batteries

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Angewandte Chemie 2024年第12期137卷

作者： Jing Tan Rui Huang Kunpeng Li Prof. Xu Yan Lin Guo Prof. Zaiping Guo Prof. Wenchao Zhang Prof. Liyuan Chai School of Metallurgy and Environment Central South University Changsha 410083 China Chinese National Engineering Research Centre for Control & Treatment of Heavy Metal Pollution Central South University Changsha 410083 China These authors contributed equally to this work and should be considered co-first authors. State Key Laboratory of Advanced Metallurgy for Non-ferrous Metals Central South University Changsha 410083 China School of Chemical Engineering and Advanced Materials The University of Adelaide Adelaide SA 5005 Australia

The recycling of critical metals from spent lithium-ion batteries represents a significant step towards meeting the enhancing resource requirements in the new energy industry. Nevertheless, achieving effective leaching of metals from the stable metal-oxygen (MO 6 ) structure of spent ternary cathodes and separation of metal products simultaneously still remained a huge challenge towards industrial applications. Herein, a competitive coordination strategy was proposed to design a novel deep eutectic solvent (DESs), which improved both leaching and selective metal recycling capacity even at high solid–liquid ratio (1 : 10). The results demonstrated that the number of hydrogen bonds in designed ternary DESs was 16.5 % higher compared to those in the binary DESs, resulting in efficient reaction kinetics to break the metals-oxygen bond. More importantly, the competing-ligand (p-toluenesulfonic acid) could preferentially enter into the first nanostructure sheath and reduce the proportion of solvated oxalic acid (OxA) from 28.36 % to 17.76 % within the nanostructure, which enable OxA molecules to enhance the coordination interaction with metal for precipitating NiC 2 O 4 ⋅ 2H 2 O product (~95.7 % purity) from spent cathodes. This work achieved impressive profitability ($16.05 per kg feedstock) and effectively reduction of GHG emissions during the recycling process, making it applicable to critical sustainability initiatives.

关键词： Spent cathode Battery Recycling Deep Eutectic Solvent Selective Recycling Nanostructure Regulation

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Cultivar-specific response of a root-associated microbiome assembly of rice to cadmium pollution

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Plant physiology and biochemistry : PPB 2025年 227卷 110128页

作者： Feng Zhang Rui Peng Yunhe Xie Xionghui Ji Saihua Liu Huidan Jiang Hunan Academy of Agricultural Sciences Hunan Cultivated Land and Agricultural Eco-Environment Institute Changsha 410125 China Longping Branch College of Biology Hunan University Changsha 410125 China Key Lab of Prevention Control and Remediation of Soil Heavy Metal Pollution in Hunan Province Changsha 410125 China. Hunan Hybrid Rice Research Center Changsha 410125 China. Hunan Academy of Agricultural Sciences Hunan Institute of Microbiology Changsha 410125 China Yuelushan Laboratory Changsha 410082 China. Electronic address: jianghuidan@***.

Rice (Oryza sativa L.) cadmium (Cd) contamination is a serious threat to global food security and human health. However, the response of rice root-associated microbiomes to Cd pollution remains unclear. This study investigate the interactions between the root-associated microbiome and plant metals using environmental and microbial analysis methods, to reveal the potential mechanisms of the root microbiomes regulating the Cd accumulation in rice. The results showed that the grain Cd concentrations of the two low-Cd accumulation (LA) cultivars were 34-46 % lower than that of the high-Cd accumulation (HA) cultivars, whereas the iron (Fe) content in the LA roots was significantly higher than that in the HA roots. The root Fe content was significantly negatively correlated with the Cd concentration of grain (R = -0.681, p < 0.05). 16S rRNA amplicon sequencing showed that rice planting significantly changed the diversity of the root-associated bacterial community and formed a unique core endophytic microbiome (such as Xanthobacteraceae and Sphingomonas) under Cd stress. LA cultivars assembled more root core microbial taxa, which promoted siderophore secretion and root Fe uptake, thereby inhibiting Cd uptake by rice. Chrome azurol S plate detection confirmed that the LA rhizosphere was enriched with 1-9-fold more siderophore-secreting microorganisms than the HA rhizosphere. This study provides new insights into the effects of root-associated microbiomes on Cd accumulation in plant and will help develop new strategies for the safe production of rice.

关键词： Cd Paddy soil Rice cultivars Root-associated microbiome Siderophore-secreting microbe Soil Fe availability

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Cathodic Hydroxide Ions Induce Tetrose Formation during Glycolaldehyde Electroreduction to Alcohols: A Potential CO2-to-Carbohydrate Pathway

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Angewandte Chemie 2025年第24期137卷

作者： Ernest Pahuyo Delmo Haichuan Zhang Jessa Vispo De Guzman Rans Miguel Nunag Lintag Juhee Jang Yao Yao Yinuo Wang Shangqian Zhu Tiehuai Li Mingguang Pan Hongming Xu King Lun Yeung Minhua Shao Department of Chemical and Biological Engineering The Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong China School of Sciences Great Bay University Dongguan 523000 China Energy Institute Chinese National Engineering Research Center for Control & Treatment of Heavy Metal Pollution and CIAC-HKUST Joint Laboratory for Hydrogen Energy The Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong China Guangzhou Key Laboratory of Electrochemical Energy Storage Technologies Fok Ying Tung Research Institute The Hong Kong University of Science and Technology Guangzhou 511458 China

The electrochemical synthesis of organic compounds from CO 2 can potentially alleviate climate change by hampering the atmospheric accumulation of greenhouse gases. The production of carbohydrates from CO 2 reduction will have promising applications for the manufacturing of valuable, multi-carbon compounds that are traditionally produced from the petrochemical or agricultural industries. In this work, we analyzed the copper-catalyzed electrochemical reduction of glycolaldehyde, a commonly observed trace CO 2 RR product that has been previously proposed as an intermediate for alcohol formation. We determine that glycolaldehyde is not the main intermediate on polycrystalline copper-based electrocatalysts that selectively produce ethanol. In an unbuffered electrolyte, the cathodic hydroxide ions produced induce the coupling of glycolaldehyde to tetroses in the solution phase, yielding a maximum glycolaldehyde-to-sugar conversion of 47.2% under ambient conditions. Using in situ infrared spectroscopy coupled with density functional theory (DFT) calculations, we show that glycolaldehyde reduction to alcohols proceeds via adsorption of its enol tautomer, η 2 (C,C)─CHOH═CHOH. Our findings not only shed light on the C 2 alcohol formation pathways during CO 2 RR, but also imply that a CO 2 electrolyzer can potentially produce C 4 carbohydrates via CO 2 reduction to glycolaldehyde followed by C─C coupling in the solution phase, with only a high local pH needed to drive the tetrose formation step.

关键词： Carbohydrate CO2 reduction Electrocatalysis Glycolaldehyde Tetrose

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Fluorine-Doped Carbon Support Enables Superfast Oxygen Reduction Kinetics by Breaking the Scaling Relationship

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Angewandte Chemie 2024年第47期136卷

作者： Jinhui Liang Lecheng Liang Binwen Zeng Binbin Feng Prof. Li Du Xiaoyi Qiu Yian Wang Prof. Huiyu Song Prof. Shijun Liao Prof. Minhua Shao Prof. Zhiming Cui Guangdong Provincial Key Laboratory of Fuel Cell Technology School of Chemistry and Chemical Engineering South China University of Technology 510641 Guangzhou China Department of Chemical and Biological Engineering and Energy Institute Chinese National Engineering Research Center for Control & Treatment of Heavy Metal Pollution The Hong Kong University of Science and Technology 999077 Hong Kong China CIAC-HKUST Joint Laboratory for Hydrogen Energy Energy Institute The Hong Kong University of Science and Technology Clear Watery Bay Kowloon 999077 Hong Kong China Guangzhou Key Laboratory of Electrochemical Energy Storage Technologies Fok Ying Tung Research Institute The Hong Kong University of Science and Technology 511458 Guangzhou China

It is well-established that Pt-based catalysts suffer from the unfavorable linear scaling relationship (LSR) between *OOH and *OH (ΔG(*OOH)=ΔG(*OH)+3.2±0.2 eV) for the oxygen reduction reaction (ORR), resulting in a great challenge to significantly reduced ORR overpotentials. Herein, we propose a universal and feasible strategy of fluorine-doped carbon supports, which optimize interfacial microenvironment of Pt-based catalysts and thus significantly enhance their reactive kinetics. The introduction of C−F bonds not only weakens the *OH binding energy, but also stabilizes the *OOH intermediate, resulting in a break of LSR. Furthermore, fluorine-doped carbon constructs a local super-hydrophobic interface that facilitates the diffusion of H 2 O and the mass transfer of O 2 . Electrochemical tests show that the F-doped carbon-supported Pt catalysts exhibit over 2-fold higher mass activities than those without F modification. More importantly, those catalysts also demonstrate excellent stability in both rotating disk electrode (RDE) and membrane electrode assembly (MEA) tests. This study not only validates the feasibility of tuning the electrocatalytic microenvironment to improve mass transport and to break the scaling relationship, but also provides a universal catalyst design paradigm for other gas-involving electrocatalytic reactions.

关键词： Break linear scaling relationship oxygen reduction reaction fluorine-doped carbon mass transport electrocatalytic microenvironment

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Corrigendum to "Peroxymonosulfate (PMS) activation by mackinawite for the degradation of organic pollutants: Underappreciated role of dissolved sulfur derivatives" [Sci. Total Environ. 811 (2022) 151421]

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The Science of the total environment 2022年 834卷 155468页

作者： Kunjie Hou Zhoujie Pi Fei Chen Li He Fubing Yao Shengjie Chen Xiaoming Li Dongbo Wang Haoran Dong Qi Yang College of Environmental Science and Engineering Hunan University Changsha Hunan 410082 China Key Laboratory of Environmental Biology and Pollution Control Hunan University Ministry of Education Changsha Hunan 410082 China. Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment Ministry of Education Chongqing University Chongqing 400045 China College of Environment and Ecology Chongqing University Chongqing 400045 China. Electronic address: fchen0505@***. School of Metallurgy and Environment Central South University Changsha 410083 China Chinese National Engineering Research Center for Control and Treatment of Heavy Metal Pollution Changsha 410083 China. Key Laboratory of Environmental Biology and Pollution Control Hunan University Ministry of Education Changsha Hunan 410082 China. Electronic address: yangqi@***.

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High-Performance Ammonia Electrosynthesis from Nitrate in a NaOH−KOH−H2O Ternary Electrolyte

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Angewandte Chemie 2024年第22期136卷

作者： Usman Bin Shahid Yongjun Kwon Yuan Yuan Shuang Gu Minhua Shao Department of Chemical and Biological Engineering Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong P.R. China Department of Chemistry and Chemical Engineering Lahore University of Management Sciences Lahore Pakistan Department of Mechanical Engineering Wichita State University Wichita KS USA Energy Institute Hong Kong Branch of the Southern Marine Science and Engineering Guangdong Laboratory and Chinese National Engineering Research Center for Control & Treatment of Heavy Metal Pollution The Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong P.R. China Guangzhou Key Laboratory of Electrochemical Energy Storage Technologies Fok Ying Tung Research Institute The Hong Kong University of Science and Technology Guangzhou 511458 China

A glut of dinitrogen-derived ammonia (NH 3 ) over the past century has resulted in a heavily imbalanced nitrogen cycle and consequently, the large-scale accumulation of reactive nitrogen such as nitrates in our ecosystems has led to detrimental environmental issues. Electrocatalytic upcycling of waste nitrogen back into NH 3 holds promise in mitigating these environmental impacts and reducing reliance on the energy-intensive Haber–Bosch process. Herein, we report a high-performance electrolyzer using an ultrahigh alkalinity electrolyte, NaOH−KOH−H 2 O, for low-cost NH 3 electrosynthesis. At 3,000 mA/cm 2 , the device with a Fe−Cu−Ni ternary catalyst achieves an unprecedented faradaic efficiency (FE) of 92.5±1.5 % under a low cell voltage of 3.83 V; whereas at 1,000 mA/cm 2 , an FE of 96.5±4.8 % under a cell voltage of only 2.40 V was achieved. Techno-economic analysis revealed that our device cuts the levelized cost of ammonia electrosynthesis by ~40 % ($30.68 for Fe−Cu−Ni vs. $48.53 for Ni foam per kmol-NH 3 ). The NaOH−KOH−H 2 O electrolyte together with the Fe−Cu−Ni ternary catalyst can enable the high-throughput nitrate-to-ammonia applications for affordable and scalable real-world wastewater treatments.

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An Overlooked Natural Hydrogen Evolution Pathway: Ni2+Boosting H2O Reduction by Fe(OH)2Oxidation during Low-Temperature Serpentinization

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Angewandte Chemie 2021年第45期133卷

作者： Han Song Dr. Xinwen Ou Dr. Bin Han Haoyu Deng Prof. Wenchao Zhang Prof. Chen Tian Prof. Chunfang Cai Prof. Anhuai Lu Prof. Zhang Lin Prof. Liyuan Chai School of Metallurgy and Environment Central South University Changsha Hunan 410083 China School of Environment and Energy Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling South China University of Technology Guangzhou Guangdong 510006 China Chinese National Engineering Research Center for Control & Treatment of Heavy Metal Pollution Changsha Hunan 410083 China Key Laboratory of Cenozoic Geology and Environment Institute of Geology and Geophysics Chinese Academy of Sciences Beijing 100029 China Beijing Key Laboratory of Mineral Environmental Function School of Earth and Space Sciences Peking University Beijing 100871 China

Natural hydrogen (H 2 ) has gained considerable attentions as a renewable energy resource to mitigate the globally increasing environmental concerns. Low-temperature serpentinization (<200 °C) as a typical water–rock reaction is a major source of the natural H 2 . However, the reaction mechanism and the controlling step to product H 2 remained unclear, which hinders the further utilization of natural H 2 . Herein, we demonstrated that the H 2 production rate could be determined by the Fe(OH) 2 oxidation during low-temperature serpentinization. Moreover, the co-existence of Ni 2+ could largely enhance the H 2 production kinetics. With the addition of only 1 % Ni 2+ , the H 2 production rate was remarkably enhanced by about two orders of magnitude at 90 °C. D 2 O isotopic experiment and theoretical calculations revealed that the enhanced H 2 production kinetics could be attributed to the catalytic role of Ni 2+ to promote the reduction of H 2 O.

关键词： Fe(OH)2 oxidation hydrogen production low-temperature serpentinization nickel water reduction

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