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T H I S A C S W E B I N A R W I L L B E G I N S H O R T L Y . . .

Slides available now! Recordings are an exclusive ACS member benefit.

Is Paper and Pulp Recycling the Solution to Our Single Use Package Problem?

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This ACS Webinar is co-produced with the ACS Green Chemistry Institute

Richard VendittiProfessor, Department of Forest Biomaterials,

North Carolina State University

David ConstableDirector, Green Chemistry Institute,

American Chemical Society


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Webinar Outline

1. Paper Industry Overview

2. Green Chemistry in the Paper Industry

3. Paper Recycling

4. Innovation and Green Chemistry Concepts in

the Paper Industry

5. Summary

Digester

Washers

Evaporators

Recovery

Boiler

Caustic

Plant

Lime

Kiln

Pulp &

Black Liquor

Weak Black

Liquor

Strong Black

Liquor

Green

Liquor

White Liquor

Lime

Mud

CaCO3

Lime

Pulp

Wash

Water

Chips

Na2S, Na2CO3

Na2S, NaOH

CaO

Brown

Pulp

Storage

Screens &

Cleaners

Bleach

Plant

Bleach

Pulp

Storage

To Paper Machine

Chipper &

Screens

Debarking

DrumLogs

Wash

Water

SteamTurbine

Generator

Power

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Objective: Demonstrate the Basic Principles of Green Chemistry in the Paper Industry

• Prevention of waste

• Maximum incorporation of reactants into product

• Minimization of hazardous products

• Safe chemicals

• Minimum Energy requirement

• Appropriate solvent

• Appropriate starting materials

• Avoid protecting group

• Use catalysts

• Biodegradable Products

• Safe Operations

Principles of Green Chemistry: Anastas and Warner

Paper Industry:

Sustainable Raw Materials

Sustainable Processes

Green Products

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1. Overview of the Paper Industry

papersciencenc state university

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Importance of Paper

Society vitally depends on pulp and paper products

Paper plays an important role in so many areas of human activity

• Communication

• Packaging

• Tissue and toweling

• Hygiene and Health Products

• Filtration

• Dissolving Pulps: cellulosic plastics

• ……

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Worldwide Demand of Paper and Paperboard

Source: RISI

In thousand tonnes

0

50,000

100,000

150,000

200,000

250,000

300,000

350,000

400,000

450,000

P&B Demand

USA

Rest of the World

China

Current total consumption is about 400 million metric tons per year Current total consumption 400 million t/yr: 1 billion tons of wood 20 billion tons of water

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Overall P&B demand dependent on GDP per capita, but relationship is country-specific

Slide Courtesy of Richard Phillips, NCSU

Source: World Bank 2018 Source: RISI 2018 Source: Author

• Well know correlation of P&B demand with GDP per capita

• Doesn’t allow country-specific predictions because of the different economic structures

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Forests allow life on earth …. Forests help humans drink, eat, and breathe

Forests lands have decreased by 33% since the pre-industrial age. (earth-policy.org)

Plantations are 7% of total forests, can provide 2/3 of the roundwood.

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Global Forests - Food and Agricultural Organization (FOA) of the

United Nations, Global Forest Resources Assessment 2010

• Forests cover 31% of total global land, 4 billion hectares

• World forests store 289 gigatonnes of carbon, decreasing by about 0.5 Gt per year

• Forests provide unrivaled ecosystem services

• Carbon sink

• Water purification

• Air purification

• Produce oxygen

• Produce soils

• Climate buffer

• Wildlife

• Social benefits

• Materials for mankind

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Forest Certification

• Certification: measures to protect water quality, biodiversity, wildlife habitat, species at risk, and forests with exceptional conservation value. Also chain of custody.

• The Sustainable Forestry Initiative (SFI) – N. America

• The Forest Stewardship Council (FSC) - Global

• More than half of forest land is certified in Canada, Europe, Scandinavian countries

• In the United States 97% of timberland certified, 29% from 3rd party (AF&PA)

• In the United States between 1990 and 2015, forest area expanded in the U. S. from 746 to 766 million acres (2.6%).

https://www.arcgis.com/apps/MapJournal/index.html?appid=dfe7da49c651424eb39a14c61c4d5f7f

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Why are we losing forest land currently?

• Fires, pest, disease, invasive species impact forest lands the most

• Forest areas are mainly lost in tropical countries via expansion of agricultural lands or fuels for burning

• Any method to promote forests is important….sustainably deriving value from forest lands promotes land being in forests

• Economically viable, sustainable forest products industry promotes forests

Source: Global Forests (Food and Agricultural Organization (FOA) of the United Nations, Global Forest Resources Assessment 2010)

https://www.arcgis.com/apps/MapJournal/index.html?appid=dfe7da49c651424eb39a14c61c4d5f7f

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• Safe chemicals





• Use catalysts


• Safe Operations

Sustainable, Renewable Wood

For the statement, “The paper industry is a positive influence in sustainably maintaining forest land”, what is your level of agreement?

Audience Survey QuestionANSWER THE QUESTION ON BLUE SCREEN IN ONE MOMENT

• Strongly agree

• Agree

• Neutral

• Disagree

• Strongly disagree

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* If your answer differs greatly from the choices above tell us in the chat!

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2. Green Chemistry at Work in the Paper Industry


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A Modern Pulp and Paper Mill

Source: Jameel, Park, Venditti, Phillips, Kirkmann

http://theadventuresofjunglejenny.com/wp-content/uploads/2011/12/botnia-paper-mill.jpg

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A marvel of chemistry, engineering, and environmental knowledge

Mass/Energy BalancesComponent BalancesChemical KineticsEquilibrium Two Phase BehaviorChemical EquilibriumSeparation EfficienciesCombustion PhenomenaMore……….

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What is Pulping ?

Middle LamellaConcentrated in lignin (glue)

140 C, High Pressure, Na2S, NaOH

• Wood Pulping ~ 4000 tonnes of wood per day

• Active chemicals are Na2S and NaOH.

• May need 20% of chemicals on wood (w/w)

• CAN NOT use chemical once time and dispose

• HOW CAN THIS BE DONE?

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Chemical Kraft Pulping Key points: uses green energy, energy sufficient often, recycles chemicals and water

Digester

Washers

EvaporatorsRecovery

Boiler

CausticPlant

LimeKiln

Pulp & Black Liquor

Weak BlackLiquor

Strong Black Liquor

Green Liquor

White Liquor

LimeMud

CaCO3

Lime

Pulp

WashWater

Chips

Na2S, Na2CO3

Na2S, NaOH

CaO

BrownPulp Storage

Screens &Cleaners

BleachPlant

Paper Machine

Chipper &Screens

DebarkingDrum

Logs

WashWater

Steam

Turbine

Power

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Green Chemistry Example 1: The Liquor Recovery cycle

Digester

Washers

Recovery Boiler

0.5 t Pulp

Chips

0.2 tons Chemicals: Na2S, NaOH

Steam

C6H12O6 + O2 = 6 CO2 + 6 H2O + HEAT

Na and S → Na2S + Na2CO3

Ca(OH)2

1 t of wood

Pulp fibers Liquor: dissolved organics + chemicals

Water

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Digester

Washers

Recovery Boiler

0.5 t Pulp

Chips


Steam

C6H12O6 + O2 = 6 CO2 + 6 H2O + HEAT


Ca(OH)2

1 t of wood


0.5 t dissolved organics0.2 t of chemicals

Water

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Digester

Washers

Recovery Boiler

0.5 t Pulp

Chips


Steam

C6H12O6 + O2 = 6 CO2 + 6 H2O + HEAT


Ca(OH)2

1 t of wood


0.5 t dissolved organics0.2 t of chemicals

Water

Na2CO3 + Ca(OH)2 → NaOH + CaCO3 (ppt)

Heat and Powerrenewable energy

60-75% energy efficient

Na2S, Na2CO3

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Green Chemistry Example 1: Chemical Recovery cycle

CausticPlant

LimeKiln

Green Liquor

White Liquor

LimeMud

CaCO3 ppt

Lime Na2S, NaOHCaO

Na2S, Na2CO3

Na2CO3 + Ca(OH)2 → NaOH + CaCO3 (ppt)

CaCO3 → CaO + CO2

Fuel

95-97% Recovery of Chemicals

2CaO +H2O → Ca(OH)2

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Green Chemistry Example 2: Enzymes as a green catalyst

Selectively react with wood components to reduce bleaching chemical required

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Green Chemistry Example 2: Enzymes as a green catalyst

Used to reduce electricity usage for

mechanical refining of fibers

Courtesy: Hubbe

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Green Chemistry Example 3: The bio-refinery concept

• A modern pulp and paper mill produces • Paper

• Pulp

• Hog fuel

• Green electricity

• Steam

• Turpentine

• Oleic, Linoleic, Palmitic Acids

• Abietic, Pimaric Acids

• More…….

• The following are also produced at pulp and paper mills• Vanillin precursors

• Adhesive precursors

• Surfactant precursors

• Fertilizers

• Biodiesel

• Naptha

• Mulch

• Much more……

UPM Biofuels

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• Safe chemicals





• Use catalysts


• Safe Operations

Biorefinery, byproducts

Multiple chemical recycle loops

Near self sufficient, renewable energy

Aqueous based reaction medium

Enzyme applications to reduce energy and chemicals

The cycles that were discussed with regards to pulping accomplish which of the following?


• Recover and regenerate chemicals

• Convert dissolved organics to heat and power

• All of the above

• None of the above

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3. Paper Recycling and Green Chemistry


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Paper and Plastic Recycling

• About 400 million tonnes of paper are produced per year

• 66% of all paper is recycled (AFPA)

• About 350 million tonnes of plastic is produced per year

• 10% of plastic is recycled (BRS)

Total Paper Used Per Year Total Plastic Used per Year12 loops of trucks 10 loops of trucks

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Paper and Plastic Recycling

• About 400 million tonnes of paper are produced per year

• 66% of all paper is recycled

• About 350 million tonnes of plastic is produced per year

• 10% of plastic is recycled (BRS)

Total Paper Discarded per year Total Plastic Discarded per Year4 loops of trucks 9 loops of trucks

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What happens to Paper and Plastic in the environment?

• Cellulosic materials are readily degraded into benign materials

• Plastic materials are not

• Results from exposure to environmental micro-organisms:

0

10

20

30

40

50

60

70

80

90

100

110

0 5 10 15 20 25 30 35 40

% B

iod

egra

dati

on

Days

Cellulose

Polyester

Imperial College London

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US Recovered and Landfilled Paper

Source: afandpa.org, 2016

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Recycled products reduce many environmental impacts vs. virgin

Note: virgin fiber is critically important to maintain adequate supplies/quality of fibers

Liner Board for corrugated boxes

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Why can we recycle paper?

• Paper strength comes from hydrogen bonds

• Paper is stronger than steel per unit mass

• Hydrogen bonds are reversible, the bonding is removed when paper is put into water

Fiber

Fiber

OH

HO

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Why can we recycle paper?

• When wetted and mechanically agitated, paper falls apart into individual fibers

• This is the basis of paper recyclingFiber

Fiber

OH

HO

OH

HOH

H

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Effects of Recycling on Paper

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Rejects and Sludges from Recycling

• Printing Writing:

• Tissue Paper:

• Corrugated box:

• Shoe/cereal box:

Some people say you can only recycle paper 7 times….estimated based on a 85% yield.Each recycle some fibers are broken into small fines that are typically washed away.

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U.S. Recovery Rate of Boxes = 93.8%

AF&PA

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Containerboard Supply Chain

Box Customer

ProductCustomer

Disposal

Recovery

Collection/Baling

Box Plant

Loss

Total Wood 43,007,744

179,350,756

“Virgin “ CBM

29,538,471

“Recycled“ CBM149,812,285

Total Containerboard 138,718,720

40,632,036

Recovery Rate

77%

OCC 138,718,720

MP 10,143,785

DLK 2,105,742

Other 6,271,587

Total Fibers 157,239,834

Wood Pulp 24,879,127

NW Pulp 257,288

RC Pulp 4,418,275

Total Fibers 29,554,689

Source: FisherSolveTM, 2018Slide courtesy

Richard Phillips, NCSU.

http://www.zimbio.com/go/KiHXBRi4xnb/http:/www.packingmaterial1.com/wp-content/uploads/2011/05/corrugated-cardboard-boxes.jpg

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How is paper recycled?

- Plastic bottles - Staples, sand

- Plastic Film - Inks -Inks, Fillers

Large Size Hydrophobicity Small Size

Large Size High and Low Density

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Recycling MOW into “Away from Home Tissue”

PulperPPM = 10,000

5,500

900

PPM = 640,

Brightness = 77%

Yield = 70%

3,700

Cleaner

Kneading

Washing

Bleaching

Screen

Washing

Did you know that recycled copy paper is cleaned to 10 ppm?

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• Safe chemicals





• Use catalysts


• Safe Operations

Paper is biocompatible

66% of paper is recycled

Collection of recovered (sorted) papers

Paper is degradable

The ability to recycle paper back into paper is MAINLY because:


• Adhesives in the old paper can be replaced by new adhesive

• Fibers never lose any strength

• Paper is held together by reversible hydrogen bonding

• Fibers never are broken in recycling

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4. Innovative and emerging green chemistry

concepts in the paper industry


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Cellulose Nanomaterials Structure

1. Siro and Plackett, 2010. 2. Turbak, 1983. 3. Dufresne, 1962 . 4. Teixeiria, 2010.

Mechanical Treatment1983 by Turbak, homogenizer, wood pulp microfibrilsApplication: thickeners in food, paints and coatings

Cellulose nanocrystals (CNC)

Chemical TreatmentAcid Hydrolysis (H2SO4)cleavage of glycosidic bonds

• Rod-shape form

• Length (200 nm) and width (20 nm)

• Mainly crystalline

• Network of long, flexible, entangled cellulose nanofibers

• Width 10-100 (nm), length (µm)

• Both amorphous and crystalline

1µm

Nanofibrillated cellulose (NFC)Microfibrillated cellulose (MFC)

200nm

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Water Vapor Transmission Rate

0

0.5

1

1.5

2

2.5

0 5 10 15 20 25 30

WV

TR

* 1

00 (

(g/m

2*d

ay)/

m)

Coating Weight (g/m2)

Beeswax

Paraf f in

Cooked Starch

MFC

LDPE

Spence, K. L., Venditti, R. A., Rojas, O. J., Pawlak, J. J., & Hubbe, M. A. (2011). Water Vapor Barrier Properties of Microfibrillated Cellulose Films. Bioresources, 6(4), 4370-4388, 2011.

Polyethylene

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NFCC 1 & 2 for Fluorochemicals Replacement

Laurel A. Schaider, Simona A. Balan, Arlene Blum, David Q. Andrews, Mark J. Strynar, Margaret E. Dickinson, David M. Lunderberg, Johnsie R. Lang, and Graham F. Peaslee, Fluorinated Compounds in U.S. Fast Food Packaging. Environmental Science & Technology Letters 2017 4 (3), 105-111 DOI: 10.1021/acs.estlett.6b00435T. H. Begley, W. Hsu, G. Noonan & G. Diachenko (2008) Migration of fluorochemical paper additives from food-contact paper into foods and food simulants, Food Additives & Contaminants: Part A,25:3, 384-390, DOI: 10.1080/02652030701513784

Studies have shown that PFOAs can migrate from food packaging into the food you eat.

Courtesy of Dr. Lokendra Pal, Forest Biomaterials, NCSU.

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High performance nanocellulose-based composite coatings for oil and grease resistance

Cellulose (2018) 25: 3377.

Coatings Kit Rating

No Coating 0

CNC 0

CNC-AKD 1

CNC-S20 2

CNC-S20-AKD 5

CNC-S20-AKD-K20 4

CNC-S20-AKD-MMT20 6

Courtesy of Dr. Lokendra Pal, Forest Biomaterials, NCSU, Tyagi, et al, Cellulose (2018).

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• Safe chemicals





• Use catalysts


• Safe Operations

Replace fluorinated compounds

Biorefinery, byproducts

Aqueous based

Renewable nanocellulose, protein, clay, wax

Replace fluorinated compounds

Cellulose based materials

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The next time you go to the grocery store, which would you prefer to use?


• Paper bags

• Plastic bags

• Reusable bags

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5. Summary


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Paper v. Plastic

• Polystyrene foam, poly coated paper, wax coated paper, solid PLA cold cups

• Functional unit: 10,000 cups

• Focus on energy, solid waste, GWP, water use

• Life cycle inventory of foam PS, Paper based, and PLA foodservice products, Franklin Associates, Plastic Food Packaging Company, 2011.

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Single use packaging…Paper or plastic?

• Paper recycled at 66%, plastic 10% (+)

• Paper recycling insfrastructure is vast and effective (+)

• Paper recycling economics better than plastics (+)

• Paper promotes forests, plastics do not (+)

• Paper degrades in the environment, plastics generally do not (+)

• Total Material in a product: Paper 2.5 times greater (-)

• Global Warming: Paper 30% less (+)

• Water Use: Paper 2 times more (-)

• Fossil Energy: Paper and Plastic Equal (=)

• Paper uses a large fraction of renewable energy (+)

• Plastic is less expensive in general (-)

• Plastics have additives that may be of concern (+)

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Section Summary

• Paper has an advantage over petroleum products in that it is renewable and biodegradable

• Petroleum products have some environmental advantages in other LCA impact categories

• In general, recycled paper has better environmental performance than virgin paper but they are both part of the same system

• Paper products consume wood and the associated lands to grow it

This is good – encourages more forests

This can have issues in developing countries if wood is not sustainably sourced

• Manufacturing and end-of-life are critical life-cycle stages in paper

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• Safe chemicals





• Use catalysts


• Safe Operations

Paper Industry:

Sustainable Raw Materials

Sustainable Processes

Green Products

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Dr. Richard Venditti,

Paper Science and Engineering,

NC State University

E-mail: [email protected]

Website: www.go.ncsu.edu/Venditti

Thanks to Dr. Byrd, Dr. Pawlak, Dr. Pal and Dr.

Jameel at NCSU for allowing the use of their slides.

Thank You!



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mailto:[email protected]

http://www.go.ncsu.edu/Venditti


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