1 Supplementary materials 2 Applications of microbial laccases: Patent review of the past decade (2009-2019) 3 Anastasia Zerva 1, Stefan Simić 2, Evangelos Topakas 1,* and Jasmina Nikodinovic-Runic 2,* 4 1 IndBioCat Group, Biotechnology Laboratory, School of Chemical Engineering, National Technical University of Athens, 5 Iroon Polytechniou Str., Zografou Campus, Athens 5 15780, Greece; 6 2 Institute for Molecular Genetics and Genetic Engineering, University of Belgrade; Vojvode Stepe 444a, 11000 Belgrade, Serbia 7 * Correspondence: [email protected]; Tel.: +381 11 397 6034 (J.N.R.); [email protected]; Tel.: +30 210 772 3264 (E.T.) 8 Catalysts 2019, 9, x; doi: FOR PEER REVIEW www.mdpi.com/journal/catalysts Catalysts 2019, 9, x FOR PEER REVIEW 2 of 8 9 Table S1. The patents cited in the main text. Appearance Year of Title Patent number Inventor (Applicant) Category in text publication Nathaniel T. Becker, Freezing point depressed solid Joseph C. Mcauliffe, Enzyme Production, 1 matrix compositions for melt WO 2019089898 A1 2019 Peyman Moslemy, Immobilization and granulation of enzymes Jared Enwei Tan, Biocatalysis Luther White (Danisco Us Inc) Wayne Ashton, Andreas J. Krouwer, Enzyme Production, Laccases and methods of use 2 US 20110302722 A1 2011 Joseph C. McAuliffe, Immobilization and thereof at low temperature Piera M. Pericu, Biocatalysis Huaming Wang (Danisco Us Inc) Huaming Wang, Enzyme Production, Laccase variants having increased 3 US 20140123404 A1 2014 Michael Ward Immobilization and expression and/or activity (Danisco Us Inc) Biocatalysis Aziz Fadli, Specific 7-amino-1,2,3,4- Zhibo Liu, Pharma / Cosmetics / 4 tetrahydroquinolines, method, and WO 2019072697 A1 2019 Céline Richardson Agrochemicals composition (L'oreal) Compositions and methods for Andrea Elsen, improving color deposit and Pharma / Cosmetics / 5 WO2019046396A1 2019 Nghi Van Nguyen, durability of color in artificially Agrochemicals Jim Singer colored hair Liu Guozhong Pretreatment process of jute or red 6 CN102086533A 2013 (Jiangsu Bauhinia Textile Textiles and fibers ramie Technology Co., Ltd.) Liu Guozhong Yao Jiangang, Zhang Zhenyao, Refining processing method of 7 CN102517648A 2012 Zhang Ximing Textiles and fibers fibrilia (Jiangsu Bauhinia Textile Technology Co., Ltd.) Catalysts 2019, 9, x FOR PEER REVIEW 3 of 8 Chen Yangmei, Jiang Yu, A kind of laccase chemical Wu Qitang, Chen Jiajin, Lignin removal and 8 modification method and its CN108823177A 2018 Qiu modification application Zhuotao, Chen Shuanna, (South China Agricultural University) Wang Zhiwei, Wu Ming, Ma Haijun, A method of true qualities Huang Huanhuan, Lignin removal and 9 mechanical pulp is prepared using CN109098025A 2018 Wang Shuangfei, modification laccase treatment bagasse Liu Xinliang, Lu Peng (Guangxi University) Sun Wei, Chen Guang, Yan Zechang, A kind of myrothecium verrucaria Su Yujie, Enzyme Production, 10 of high yield laccase and CN109868224A 2019 Wang Gang, Immobilization and application Chen Huan, Biocatalysis Yu Yu (Jilin Agricultural University) Guan Zhengbing, The CotA laccase and its Enzyme Production, Xu Kaizhong, 11 application that a kind of catalytic CN109439635A 2019 Immobilization and Liao Xiangru efficiency improves Biocatalysis (Jiangnan University) Zhang Jie, Enzyme Production, A method of enzyme is recycled in 12 CN109652386A 2019 Zhang Jiaying, Immobilization and catalysis reaction Xu Hui, Biocatalysis Catalysts 2019, 9, x FOR PEER REVIEW 4 of 8 Li Fukun, Cheng Zhongqi (Chongqing Technology and Business University) Enzyme-metal hybrid nanoflowers Sanjay K.S. Patel, Seong Hun Yeong, Enzyme Production, 13 and its application in repeated KR 20190033780A 2019 Jinglin Li, Jung Kul Lee (Univ Immobilization and batch decolorization of dyes Konkuk Ind Coop Corp) Biocatalysis Zhang Mei, Zhang Yimei, Preparation method of poly(methyl Lai Wei, Enzyme Production, methacrylate) coated carboxyl 14 CN107988196A 2018 Wu Panpan, Immobilization and carbon nanotube immobilized Wang Liqun Biocatalysis laccase (North China Electric Power University) Jung Bae Kim, Hansol Kim (Korea Enzyme Production, Enzyme-porous carrier composite 15 KR 20180041065A 2018 University Industry- Academic Immobilization and and manufacturing method thereof Coop Fondation) Biocatalysis Method for biomimetic synthesis of Wang Meiyin, Enzyme Production, 16 nano zirconium dioxide CN107858344A 2018 Wu Huimin Immobilization and immobilized laccase (Fuzhou University) Biocatalysis Sheng-Chi Wu, Method for preparing bacterial Enzyme Production, Sian-Ming Wu, 17 cellulose adsorbing enzyme and TWI622646B 2018 Immobilization and Feng-Min Su, product thereof Biocatalysis (Fooyin University) Guan Zhengbing, Modified diatomite carried Zhou Wen, Enzyme Production, immobilized spore laccase as well Liao Xiangru, 18 CN105063008A 2018 Immobilization and as preparation method and Cai Yujie, Biocatalysis application thereof Chen Kang (Jiangnan University) Catalysts 2019, 9, x FOR PEER REVIEW 5 of 8 Stéphane Grelier, Henri Cramail, Audrey Llevot, Enzyme Production, New process for preparing 19 WO2016050988A1 2016 Stéphane Carlotti, Immobilization and biphenyl compounds Etienne Grau Biocatalysis (Université De Bordeaux, Institut Polytechnique De Bordeaux, CNRS) Method for preparing hyaluronic Qi Jicheng, Pharma / Cosmetics / 20 acid substitute through oxidizing CN104745662A 2015 Yin Yunbei (Tianjin University of Agrochemicals chitosan by laccase-TEMPO system Science and Technology) Liu Ying; Liu Guohong; Wang A kind of cotton fabrics and its pre- 21 CN109722908A 2019 Guan; Chen Jie; Zhou Ying (Wuhan Textiles and fibers treating method Sunhy Biological Co. Ltd Sun Yi, Low-temperature oxygen Xu Yu, 22 bleaching activator for pure cotton CN108642854A 2018 Textiles and fibers Zhang Wei fabric (Sun Yi) Alex Sivan, Compositions and methods for Bioremediation and 23 WO2014167562A1 2014 Amir Aharoni, biodegrading plastic Detoxification (B.G Negev Technologies Ltd.) Stephane C. Corgie, Mesoporous catalysts of magnetic Patarawan Kahawong, nanoparticles and free-radical- Bioremediation and 24 WO2012122437A2 2012 Emmanuel Giannelis, producing enzymes, and methods Detoxification Larry P. Walker of use (Cornell University) Nina Mußmann, Timothy O'Connell, Detergents with improved Daniela Herbst, 25 detergent power, containing at US20180127687A1 2018 Inken Prueser, Detergents least one laccase Ralf G. Berger, Diana Linke, Christoph Behrens Catalysts 2019, 9, x FOR PEER REVIEW 6 of 8 (Henkel AG and Co KGaA) Nina Mußmann, Timothy O'Connell, Thomas Weber, Detergent containing at least one Mareile Job, 26 US20170267947A1 2017 Detergents laccase as a dye-transfer inhibitor Hendrik Hellmuth, Michael Strotz, Inken Prueser (Henkel AG and Co KGaA) Hu Ping, Preparation method and Zhou Xinlin, application of two-dimensional 27 CN103499625A 2015 Wu Qingsheng Sensors and biofuel cells nano rare earth borate laccase (Tongji University) sensor A kind of preparation of the Yu Jinghua, 28 electrochemical sensor shown with CN110068570A 2019 Sun Jianli, Sensors and biofuel cells instant visualization colorimetric Li Li (Ji Nan University) Method for preparing Zhang Chong, Bu Guojian, Zhang protein/pectin/chitosan composite Xiajoian film by using thermostable Polymers and 29 CN109111584A 2019 (Nanjing Agricultural University, recombinant bacterial laccase, and biopolymers Taixing Dongsheng Bio Tech Co. product thereof, and applications Ltd.) of product A kind of preparation method of Liu Shiming (Quanjiao Xiangrui Polymers and 30 automobile instrument panel CN109096736A 2018 Plastic Co., Ltd.) biopolymers sealing element Catalysts 2019, 9, x FOR PEER REVIEW 7 of 8 Lacquer for paper base lacquer Meng Meilin, Meng Yucun, Sheng 31 painting and preparation method CN 109627825 2019 Rong (Anhui Polytechnic Paint and coatings thereof University) Preparation method of thermal- Lu Na (Changzhou City Richen 32 CN 109735175 2019 Paints and coatings insulation coating for exterior wall Decoration Materials Co., Ltd.) 10 11 Table S2. Comparison of recent laccase-related journal publications and patents across categories. Scientific publicationsa Patents last decadeb Number of papers Number of patents Category Category (%) (%) Lignin removal and Bioremediation 29 20 modification Biofuel Biochemistry and 22 15 cells/Biosensors Biocatalysis Pharma/ Cosmetics/ Textile 20 13 Agrochemicals Pulp and paper 11 Textiles and fibers 11 Food 10 Bioremediation 10 Organic synthesis 4 Food and beverages 8 BIofuels 2 Detergents 8 Biofuel cells/ Fiberboards 0.7 7 Biosensors Plastics and Cosmetics 0.7 4 biopolymers Paints 0.3 Paints and Coatings 2 Miscellaneous 2 12 a Mate and Alcalde, [57]. b SciFinder database (2008-2019). 13 © 2019 by the authors. Submitted for possible open access publication under the terms and conditions of the Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/). 14 Catalysts 2019, 9, x; doi: FOR PEER REVIEW www.mdpi.com/journal/catalysts .